Solar Energy Materials & Solar Cells 257 (2023) 112347

Contents lists available at ScienceDirect

Solar Energy Materials and Solar Cells

journal homepage: www.elsevier.com/locate/solmat

Recent progress on transparent and self-cleaning surfaces by

superhydrophobic coatings deposition to optimize the cleaning process of
solar panels
Brahim Nomeir a, b, *, Sara Lakhouil b, c, Sofia Boukheir b, Mustapha Ait Ali a, Sanae Naamane b
a
Molecular Chemistry Laboratory, Unit Coordination and Catalysis Chemistry, Cadi Ayyad University, Faculty of Sciences Semlalia (UCA-FSSM), B.P. 2390, 40000,
Marrakech, Morocco
b
Moroccan Foundation for Advanced Science Innovation and Research (MAScIR), Rue Mohamed Al Jazouli, Rabat, Morocco
c
Mohammed V University, Mohammadia School of Engineers (EMI), Avenue Ibn Sina B.P. 765 Agdal, Rabat, Morocco

A R T I C L E I N F O A B S T R A C T

Keywords: Superhydrophobic transparent coatings have recently gained significant attention in the solar energy field due to
Superhydrophobic coatings their ease of preparation, low cost, self-cleaning process, and high effectiveness in reducing dust adhesion to the
Self-cleaning surface. However, very few journals have addressed the application of self-cleaning coatings for the solar energy
Solar panels
field due to its complexity. The transparency and the roughness responsible for the self-cleaning feature are two
Transparency
Surface science
contradictory parameters; Increasing one parameter strongly implies a decrease in the other, Moreover, the
Roughness durability of the coatings is also considered as an essential parameter for their industrial-scale acceptance, as
solar panels are exposed to highly aggressive environments. Therefore, studying superhydrophobic coatings
oriented for solar applications can be challenging. Most reviews reported in the literature provided limited in­
formation on the choice of materials, deposition techniques, and synthesis protocols of transparent and super­
hydrophobic coatings.
Several reviews have addressed the topic of superhydrophobic coatings, which have various applications such
as water/oil separation, anti-ice, anti-biofouling, self-cleaning and more. However, there are not many reviews
that specifically focus on the development of superhydrophobic coatings for solar applications. This is mainly due
to the transparency constraint required for the solar applications, making this topic particularly challenging. In
the past five years, only five reviews have been published on this subject.
In this review, we discuss in detail the impact of solar panel dust accumulation and its impact on their effi­
ciency. Then, we discuss the principle of superhydrophobicity and self-cleaning as well as the principle of
transparent coatings.

Abbreviations: CAH, Contact angle hysteresis; UV, Ultraviolet; J, joule; F2O3, Iron oxide; SiO2, Silicon dioxide; CaO, Calcium oxide; Al2O3, Aluminum oxide; PV,
Photovoltaic; PCE, Power conversion efficiency; EDS, Electrodynamic Screen; rpm, revolution per minute; TiO2, Titanium dioxide; CuO, Copper Oxide; THF,
Tetrahydrofuran; PU, Polyurethane; PDMS, Polydimethylsiloxane; PS, Polystyrene; EtOH, Ethanol; PVC, Polyvinyl chloride; ZnO, Zinc oxide; OH, Alcohols; PMMA,
Poly(methyl methacrylate); PTMS, Trimethoxypropylsilane; MTMS, Trimethoxymethylsilane; NH4F, Ammonium fluoride; PFOTS, Perfluorooctyl trichlorosilane;
TOS, Triethoxyoctylsilane; CVD, Chemical vapor deposition; PFTS, Perfluorodecyltrimethoxysilane; PFA, polyfurfuryl alcohol; PCBTF, Parachlorobenzotrifluoride;
ODA, Octadecylamine; HMDS, Hexamethyldisilazane; HDTMS, Hexadecyltrimethoxysilane; IPA, Isopropyl alcohol; OTS, Octadecyltrichlorosilane; TEOS, Tetraethyl
orthosilicate; ODTMS, Octadecyltrimethoxysilane; NaCl, Sodium chloride; NaOH, Sodium hydroxide; SEM, Scanning electron microscopy; FAS, Heptadecafluoro-
1,1,2,2-tetrahydrodecyl triméthoxysilane; PET, Polyethylene terephthalate; PFPE, perfluoropolyether; CF4, Tetrafluoromethane; Ar, Argon; FEP, Fluorinated
ethylene propylene; Tg, Glass transition temperature; Tf, melting temperature; PUA, Polyurethane-acrylate; NH4OH, Ammonium Hydroxide; H2O2, Hydrogen
peroxide; PVDF, Polyvinylidene fluoride; HFP, hexafluoropropen; MTCS, methyl trichlorosilane; PVB, Polyvinyl butyral; SnCl2, stannous chloride; AgNO3, Silver
nitrate; DMF, Dimethylformamide; DMAc, Dimethylacetamide; OPV, Organic photovoltaic; PTFE, Polytetrafluoroethylene; AACVD, Aerosol-assisted chemical vapor
deposition; MPS, 3-Methacryloxypropyltrimethoxysilane; POTS, 1H, 1H, 2H, 2H perfluorooctyltriethoxysilane; APTES, Aminopropyltriethoxysilane; TMODS, tri­
methoxyoctyldecylsilane; PECVD, chemical vapor phase assisted by plasma; KH560, glycidoxypropyltrimethoxysilane; ATRP, Atom transfer radical polymerization;
CuBr, Copper(I) bromide; PFMA, poly(2-perfluorooctylethyl methacrylate); SHS, Superhydrophobic surface; SLIPS, Slippery liquid-infused porous surface; NaPFO,
Sodium monofluorophosphate.
* Corresponding author. Molecular Chemistry Laboratory, Unit Coordination and Catalysis Chemistry, Cadi Ayyad University, Faculty of Sciences Semlalia (UCA-
FSSM), B.P. 2390, 40000, Marrakech, Morocco.
E-mail address: [email protected] (B. Nomeir).

https://doi.org/10.1016/j.solmat.2023.112347
Received 11 October 2022; Received in revised form 18 April 2023; Accepted 22 April 2023
Available online 12 May 2023
0927-0248/© 2023 Elsevier B.V. All rights reserved.
B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

In this review, we aim to address this gap in knowledge by discussing in detail the impact of dust accumulation
on solar panel efficiency, as well as the principles of superhydrophobicity, self-cleaning, and transparent
coatings.

1. Introduction For domestic installations, even thought it may only require cleaning
and rinsing of the setup, this work performed at height on a roof can pose
Since 1970, energy consumption has experienced very significant a danger for a non-professional. Moreover, using cold water on a hot
growth following the industrial revolution, which is based on the use of panel can lead to the risk of scratches or thermal shock. To address these
fossil resources [1]. These resources are exhaustible, limited and can issues, superhydrophobic coatings have recently emerged as more
cause environmental problems such as global warming. Therefore, im­ practical alternative solution. These coatings are characterized by their
provements and innovations are required to address their issues. For this self-cleaning nature [15], which reduces the accumulation of dust [ [16,
reason, the majority of research is directed towards solar energy. It is 17]], lowers the cleaning cost, maintains optimal performance, and
well known that the sun provides almost 5 × 1024 J of energy each year, ensures the durability of the panels for a long time [18].
making it the most powerful renewable resource due to the abundance It is well known that superhydrophobic surfaces are characterized by
of its light throughout the year on the earth. It can then be a good two essential parameters: firstly the slip angle which is less than 10◦ , and
alternative, using photovoltaic panels to convert solar energy into secondly, the contact angle with water which must be greater than 150◦ .
electrical energy (Fig. 1) [ [2–4]]. This character necessarily depends on the union of two factors. On the
Solar panels allow the generation of energy through a relatively one hand the chemical nature of the surface and its polarity, which must
economical, non-polluting process, and with very high efficiency. be hydrophobic. On the other hand the geometry of the surface requires
However, solar panels are subject to several degrading factors, such as having a nanostructure or a microstructure to increase its roughness
corrosion, ultraviolet rays (UV), and temperature[ [6,7]]. Additionally, until it is able to repel the droplets of water, which makes the surface
solar panels, both thermal and photovoltaic, are subject to weather that non-wetting [ [19,20]]. Due to this unique property, superhydrophobic
vary throughout the year. During the winter season, for instance, a large coatings find applications in many other fields [21], besides the field of
amount of dust is deposited on the surface of solar panels due to the solar energy [22], such as water/oil separation [ [23,24]], anti-icing [
effect of wind. The average rate of dust accumulation varies from 1 to 50 [25,26]], textiles[ [27–29]], civil engineering [30], electric power [31],
mg/m2 per day and 150–300 mg/m2 per day [8,9]. Without cleaning, energy storage [32], heat dissipation in electronic devices and vapor
the buildup of dust, bird droppings and soils on the panels surface acts as condensation [33].
a barrier, hindering the irradiation of sun rays on the panels, which Nature presents many superhydrophobic and self-cleaning surfaces
results in reduced performances and production losses [ [10,11]]. [34], such as sharkskin [35], rice leaf [36], butterfly wings [37], and
Studies conducted by Mazumder et al. [12] and Elminir et al. [13] have lotus leaf [38]. Inspired by nature, several efforts have been made to
shown that a dust layer of 4g/m2 can lead to a decrease in solar yield of understand the mechanism controlling the surfaces wettability [ [39,
up to 40%. Although rain may offer a natural cleaning solution for the 40]]. In 1805, Young showed his equation for measuring the contact
installations, in many cases it cannot replace regular cleaning [14], angle with water [41], which is valid only for smooth surfaces. In 1936,
especially for installations in desert areas that requires frequent cleaning Wenzel showed his model, but he took into account the effect of
to ensure high energy production efficiency. roughness on the contact angle [42]. In 1944, Cassie and Baxter pro­
However, the cost of cleaning is a crucial parameter that must be posed another model that takes into account the effect of accounting for
taken into and should not exceed the amount saved by the installation. surface heterogeneity [43].

Fig. 1. Evolution of total solar energy installed capacity (1996–2021) [5].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

Today several manufacturing techniques have been developed, such capillary, gravity, electrostatic, and van der Waals, depending on the
as the method of electrospinning [ [44,45]], sol-gel [ [46,47]], type of exposure environment. For instance, in high humidity environ­
spin-coating [ [48,49]], spray-coating [ [50,51]], dip-coating [ [52,53]], ments, capillary adhesion force was found to dominated between dust
plasma [ [54,55]], chemical vapor deposition [56], physical vapor and PV panels, while in the dry environment, Van Der Wals force was
deposition [ [57,58]], lithography [ [59,60]], polymerization [61], and dominant [69].
other techniques [62]. Despite this strong evolution, the application of To avoid the accumulation of dust, several cleaning techniques are
superhydrophobic coatings in the field of solar energy remains the most used, generally classified into three categories.
challenging. This is because it requires not only superhydrophobicity
but also two other essential properties, namely high transparency and - Manual cleaning is relatively primitive technology that requires high
excellent chemical and mechanical resistance to improve the durability labor costs and a large amount of water. This type of cleaning can be
of the coatings and increase their lifespan. It is well-known that performed in several ways. For example, tap water can be used to
increasing a surface roughness leads to an increase in super­ clean PV panels, but its effectiveness is limited when it comes to
hydrophobicity, but it has the opposite effect on transparency [63]. removing fine particles. Another method involves using water under
Therefore, finding a balance point that allows manufactures to create a high pressure, which is very effective but not suitable for desert
superhydrophobic coating that is mechanically stable and highly zones due to the high amount of water required. Moreover, these two
transparent requires additional advanced studies. techniques can lead to the production of stains after air-water drying,
In this review, we discuss the latest studies on self-cleaning super­ which negatively impacts yield. Another classic cleaning method
hydrophobic coatings for solar energy applications in detail. Our dis­ involves the use of soft brushes and special agents, but this cleaning
cussion covers theory, preparation, properties, applications, and process is time-consuming. Due to the higher frequency of manual
challenges to provide a comprehensive understanding of the latest cleaning, which requires at least once a week, the cost of cleaning
trends in superhydrophobic coatings and their applications in this field. more than doubles compared to cleaning by machines. The reason
We also highlight the most commonly used techniques that are of sig­ why manual cleaning is not the best choice is that it is very
nificant importance in the field of superhydrophobic coatings for solar expensive.
energy applications. First, we explain the effect of dust accumulation - Active cleaning, refers to a cleaning technology that removes dust
and the principles of superhydrophobicity and self-cleaning. The next using electrical equipment, including cleaning robots such as those
part is devoted to transparency and durability, followed by the design of proposed by Parrot et al. [77]. in their work, a 36 kg cleaning robot
superhydrophobic coatings. Finally, we discuss the manufacturing moves on the frame of the solar panels using silicone rubber brushes
techniques suitable for the fabrication of superhydrophobic surfaces for with a brush rotation speed of 120 rpm, which causes cleaning by
solar energy applications. abrasion on the panel surface. In another work, Antonelli et al. [78]
developed a waterless solar cell cleaning robot using two brushes
2. Dust accumulation and self-cleaning contained in both sides of the robot. Another active cleaning strategy
known as Electrodynamic Screen (EDS) has been widely used [79].
2.1. The impact of dust on energy efficiency This technique involves using two parallel electrodes with a thin film
made of a transparent and dielectric material, which is applied on the
The exposure of the solar panels to the external environment puts surface of the solar panels. By supplying electricity to the electrodes,
them in a direct contact with several degrading factors continuously and an electric field is generated that charges the dust particles. Under
for extended periods of time. During certain seasons of the year, wind the effect of the electric field, the charged particles move towards the
speed and direction cause dust particles to move on the surface of edge of the panels, leading to the elimination of dust. This technique
photovoltaic (PV) or thermal panels. This movement can result in the has an efficiency that can eliminate up to 90% of the dust, making it
destruction of surface morphology through erosion or the formation of a ideal for regions with water shortage. However, it is important to
dust film that prevent sunlight from reaching the panel surface. In both note that producing electricity between the electrodes requires
cases, the energy efficiency of the panels is negatively impacted consuming part of the energy produced by the photovoltaic panels.
(Table 1). The rate of dust accumulation is influenced by several pa­
rameters including the type of dust, panel orientation, wind direction, Compared to manual cleaning techniques, active cleaning techniques
and chemical composition of the dust particles. A large number of have three main advantages: they save water resources, do not damage
studies have been conducted to investigate the particle size distribution the surface of PV panels, and are controlled by a computer system.
and chemical composition of particles [ [64–67]]. Generally, the parti­
cles size varies between a few millimeters to a hundred millimeters, and - Passive cleaning, this technique consists of using a superhydrophobic
they consist of various oxides, such as iron oxide (Fe2O3), Silicon di­ or superhydrophilic coating[ [16,80]] that is deposited on the glass
oxide (SiO2), Calcium oxide (CaO), and Aluminum oxide (Al2O3). Ac­ of the solar cells. These coatings allow the elimination of dust or any
cording to a study by Tanesab et al. [68], it was observed that small organic molecules deposited on the surface by the principle of ’
particles are distributed in a much more uniform manner on the surface self-cleaning. Superhydrophilic surfaces are characterized by a con­
of PV panels, which has a significant impact on energy production. tact angle lower than 10◦ , which causes water droplets to spread
Additionally, the initial adhesion of dust to the cell surface occurs completely on the surface due to the strong adsorption of the surface.
through a combination of the interactions of various forces, including Super-hydrophilic coatings have a better affinity with water, which
allows them to penetrate the interface between the glass surface and
Table 1 the dust, spread over the glass surface, and remove the dust layer. In
Effect on PCE due to soiling at different locations. contrast, superhydrophobic coatings are based on another principle.
After a drop is deposited on the surface, the drop assumes a spherical
Location Reduction on Power conversion efficiency (PCE) References
shape due to the water repellency of the surface. Thereafter, the
Bahrein 40% in 1 year [70] spherical drop quickly slides down the surface and removes dust.
India 13% in 1 month [71]
Iraq 40% in 1 year [72]
Italy 6.9% in 1 year [73] The passive cleaning method is characterized by a very simple
USA 23% in 16 months [74] cleaning process and low cost compared to other cleaning methods.
Pakistan 20% in 1 year [75] However, the self-cleaning mechanisms for superhydrophilic surfaces
Quatar 10% in 6 month [76]
requires a significant amount of water to spread over the entire surface,

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

making it unsuitable for water-scarce regions. In contrast, super­

hydrophobic coatings have a strong self-cleaning ability due to their
unique mechanism, which requires only a small amount of water to
clean surfaces. This makes them suitable for use in all conditions,
including water shortage areas. Due to this advantage, super­
hydrophobic coatings superhydrophobic coatings have garnered atten­
tion from researchers as an alternative solution to other methods.

2.2. Superhydrophoby and self-cleaning

When a drop of water falls from a tap or a drop of rain finds itself in
the air, it adopts a spherical shape due to the imbalance of the forces
applied. The water molecules that are at the interface are not sur­
rounded by the same molecules on all sides, resulting in a greater liquid-
liquid attraction force than that of liquid air. This generate an internal
pressure, causing the water droplet to adopt a spherical shape to mini­
mize contact with external medium. However, when this drop of water
falls on a solid substrate, the adopted shape is determined by the surface
roughness, the compositions of the surface, and the interaction of the
Fig. 3. The variation of the contact angle as a function of the quantity of
water molecule with the interfaces (liquid-solid, liquid -vapor, solid- ethanol added [82].
vapor) [40]. Generally the wettability behavior of surfaces can be
classified into four groups based on the contact angle with water θ:
- Phase separation is a technique used to create superhydrophobic
superhydrophobic, hydrophobic, hydrophilic, and superhydrophilic, if
surfaces. It involves the solubilization of a polymer in a solvent,
θ > 150◦ , 90◦ < θ < 150◦ , 10◦ < θ < 90◦ , and θ < 10◦ , respectively [62].
followed by the addition of a non-solvent, such as ethanol, to the
When the drop of water moves on a superhydrophobic surface, it
reaction. The combination of tetrahydrofuran (THF) as a solvent and
assumes a spherical shape with a thin film of air appearing between the
ethanol as a non-solvent is commonly used in this technique. When
drop and the surface. This prevent the drop from penetrating the surface
the non-solvent is added to the solution, the molecules of the non-
due to limited interaction and contact. To qualify as a self-cleaning
solvent diffuse into the solution and create a thermodynamically
superhydrophobic surface, it must meet two conditions: a contact
unstable system. This instability leads to the division of the solution
angle greater than 150◦ and a sliding angle less than 10◦ . The latter
into two phases: a phase rich in polymer, which will generate a
condition allows the drop of water to glide effortlessly across the sur­
matrix structure, and a polymer-poor phase, which will be respon­
face, carrying away dust and cleaning the surface. (See Fig. 2).
sible for creating pores. The combination of the two structures, the
To obtain a superhydrophobic surface, two conditions must be ful­
matrix and pores, allows for the creation of a hierarchical
filled. Firstly, the surface must have a hierarchical nanostructure that
morphology. This morphology is responsible for the super­
can trap air, resulting in very high roughness. Secondly, the chemical
hydrophobicity of the surface. Superhydrophobic surfaces have high
structure of the surface must be hydrophobic with low surface energy
water contact angles and low sliding angles, which make them highly
[24]. When a drop of water is deposited on a superhydrophobic surface,
water-repellent. Overall, phase separation is a useful technique for
the trapped air between the microstructures pushes the drop of water,
creating superhydrophobic surfaces with a hierarchical morphology
preventing its penetration. As a result, the drop adopts a spherical shape
[85]. And it should be noted that the amount of non-solvent added
and remains deposited only on the asperities with a very limited contact
plays a very important role in controlling the obtained morphology.
surface. Due to its hydrophobic character, there is no possibility of
The typical polymers used for the manufacturing of super­
making hydrogen bonds between the drop of water and the surface, and
hydrophobic suspensions are Polydimethylsiloxane (PDMS) [86],
therefore it does not stays on the surface, allowing the drop to move
Polyurethane (PU) [ [87,88]], Polystyrene (PS) [ [89,90]]. Soheil
across the surface easily.
Piltan et al. [91] fabricated a polystyrene-based superhydrophobic
Furthermore, it is possible to manufacture superhydrophobic coat­
coating by the phase separation method using THF as a solvent and
ings even in a dry environment, using photocatalytic molecules that
water as a non-solvent. In the experimental protocol, the polystyrene
degrade molecules and dust under the effect of light. Nanoparticles of
polymer was dissolved in THF. Then, SiO2 nanoparticles were added
Titanium dioxide (TiO2) [83], Copper Oxide (CuO) [84].
to the polystyrene solution, and finally an amount of ethanol (EtOH)
was added to the PS solution. It was found that the absence of
3. The preparation of superhydrophobic formulations
non-solvent generated more superhydrophobicity, which emphasizes
the importance of this step in producing superhydrophobicity. In
There are several methods for preparing superhydrophobic coatings.
another work, Robert Brown et al. [82] reported a simple protocol
for synthesizing a superhydrophobic coating from polyvinyl chloride

Fig. 2. Comparison between cleaning of: (a) uncoated glass and (b) glass coated with a superhydrophobic coating [81].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

(PVC) using a phase separation method without the need to use hydrophobic nanoparticles on a substrate can lead to the generation of
nanoparticles. In the first step, the PVC was solubilized in THF, and superhydrophobicity. However, it does not allow obtaining sufficiently
then a series of samples was prepared with different amounts of durable surfaces, especially for coating deposition techniques such as
ethanol added to create the phase separation process. The final spin-coating, dip-coating, spray-coating. In order to improve the dura­
products were then applied to glass slides by spin-coating. They bility of coatings on substrates, the most common way is to prepare a
studied the effect of the concentration of added ethanol on the sur­ suspension of inorganic nanoparticles in combination with a polymer
face contact angle. The results showed that superhydrophobicity was resin, such as polypropylene [108], polystyrene [ [90,109]], poly­
obtained only when the concentration of ethanol added to the PVC urethane [26], Polyvinyl chloride [110], Polyphenylene sulfide [111].
matrix was 70% (see Fig. 3). it was noticed that the addition of Nanoparticles enable the creation of a rough surface with low energy,
ethanol generates the formation of pores, which increases the surface while the resin facilitates the adhesion of the nanoparticles to the sub­
roughness of the surface and consequently the superhydrophobicity. strate and improves the durability of the coatings. They also provide
For the percentages of 60% and 80% (v/v), the surface presents pores new properties in addition to superhydrophobicity on the surface, such
of 1 mm and 5 mm, respectively, whereas for the concentration of as the use of PDMS to enhance chemical and thermal stability, and the
70%, it allows obtaining pores of 2 mm, which has been the ideal for use of Polyvinylidene fluoride (PVDF) to improve UV resistance. It is
obtaining a sufficient roughness to produce superhydrophobicity. important to note that to improve the durability of the surfaces, the
This specific surface roughness generated the superhydrophobicity. resins must have dual compatibility with the chemical nature of the
substrate and at the chemical nature of the surface of the nanoparticles.
-The suspensions of nanoparticles: to achieve the two conditions of The deposition of a nanoparticle/resin nanocomposite coating can be
superhydrophobicity, high roughness and low surface energy, achieved by three methods: The first method involves depositing a layer
several studies have focused on the preparation of nanoparticles that of resin followed by the deposition of the nanoparticles [17]. The second
are deposited onto a substrate using deposition methods. The uni­ method involves depositing a suspension of a mixture of resin with the
form deposition of nanoparticles enables the creation of a hierar­ nanoparticles prepared in a solvent [15]. The third method consists of
chical morphology with micro and nanostructures that can trap the first depositing a layer of the nanoparticles followed by a deposit of a
air. Inorganic nanoparticles such as SiO2, ZnO, TiO2, CuO are polymer resin [92]. It should be noted that the concentration of the resin
commonly used due their desirable physical and chemical properties relative to the nanoparticles plays an important role in controlling the
including resistance to high temperatures, resistance to UV rays, high properties of surface wettability. It has been observed that increasing the
hardness, wear resistance, and good visible transmittances. Nano­ amount of the resin can make the surface less hierarchical, which can
particles are usually prepared through the sol-gel method from increase the slip angle [112].
metallic precursors, but this technique produces hydrophilic nano­ Solar energy applications require coatings with too high a lifespan.
particles with hydroxyl groups on their surfaces. Direct use of hy­ Although the use of resin has improved the durability of coatings,
drophilic nanoparticles can only increase surface roughness but superhydrophobic nanocomposite coatings cannot always meet the
cannot generate superhydrophobicity due to the high surface energy. needs of the application due to the loss of superhydrophobicity caused
To reduce surface energy, various surface modification techniques by mechanical and chemical damage. To address this issue, have
have been developed such as using hydrophobic agents or plasma recently turned to using polymers with self-healing properties, such as
treatments. These techniques modify the surface chemistry of the PDMS [113], PMMA [114], These polymers can maintain super­
nanoparticles, making them more hydrophobic and reducing their hydrophobicity even after mechanical damage by reforming a new
surface energy. Ultimately, the deposition of these modified nano­ surface after the chemical and morphological composition of the initial
particles on a substrate can create superhydrophobic surfaces that surface has been destroyed by external factors, such as temperature, UV,
have practical applications in self-cleaning coatings, anti-corrosion plasma.
coatings, and microfluidics. There are two strategies for rendering
nanoparticles hydrophobic. The first strategy involves the deposition 4. Superhydrophobicity and transparency
of nanoparticles followed by a deposition of a hydrophobic material
on the surface [92]. The second strategy involves the functionaliza­ Transparency is an indispensable factor in the application of solar
tion of the surface of the nanoparticles using hydrophobic molecules panels. However, from the point of view of surface roughness, super­
to replace the OH functions with hydrophobic functions. This can be hydrophobicity, and transparency are two competitive properties. It is
achieved using either fluorinated molecules such as Polytetra­ well known that increasing roughness leads to increasing super­
fluoroethylene [93],perfluoroalkyltriethoxysilane [94], per­ hydrophobicity, while transparency decreases accordingly due to light
fluorodécyltrichlorosilane [95] … acid grafting such as butyric acid scattering, which can come both from the film surface (roughness) and
[96], caproic acid [97], palmitic acid [98] … organosilane grafting inside the film (the presence of pores and grain boundaries scatter light).
such as Triethoxymethylsilane [99], Octadecyltrichlorosilane [ [100, Assuming that the roughness of a surface was created by spherical
101]], Trimethylethoxysilan [102], hexamethyldisilazane [ [103, nanoparticles and dielectrics which allow for the redirection of incident
104]] … or else polymerization of hydrophobic monomers on the light, two scattering theories are often applied to study light scattering:
surface of the nanoparticles such as perfluorooctylethyl methacrylate Rayleigh scattering and Mie scattering. The relationship between
[105], vinylidene fluoride [106]. wavelength and particle size is a very important parameter for classi­
fying scattering patterns. Rayleigh scattering is an elastic scattering of
The rate of functionalization is a crucial factor in controlling the light, occurs when the particle size is much smaller than the wavelength
wetting properties of the surface [106]. Total functionalization of the of light (<1/10 λ). The intensity of Rayleigh scattering radiation be­
surface of the nanoparticles can result in the complete absence of active comes more important as the ratio of particle size to wavelength in­
functions, which can react and bond with the surface. On the other hand, creases [115].
partial functionalization can preserve large hydrophilic areas that can When light passes through a surface, when the wavelength of the
retain water and prevent slippage. Additionally, the surface wettability, light is greater than the roughness of that surface. The intensity of light
is influenced not only by the rate of functionalization but also by the size is expressed by:
of the particles [107]. It is worth nothing that using large nanoparticles
I /I0 ∞ (1 / R2) (d6 / λ4) (1)
increases the contact area between the drop and the surface, leading to
an increase in the slip angle. Where λ is the wavelength of the incident light, d represents the
It has been proven in several studies that the deposition of

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

diameter of the particles, R represents the distance between the particle speed (Fig. 4- a). This technique is reproducible and allows for the for­
and the detector, and I0 corresponds to the intensity of the incident light. mation of controllable thicknesses. However, it does result in some
It is well known that the visible spectrum ranges from 380 to 780 nm. material waste and can only be applied to flat substrates.
For examples, if we consider a particle of size 100 nm and the incident The dip-coating technique involves immersing the substrates in a
light with a wavelength of 520 nm, equation (1) becomes: coating suspension and then withdrawing them at a constant speed
(Fig. 4- b). This technique can be applied to substrates of different shapes
I /I0 ∞ 13.67 nm2 (1 / R2) (2) and allows for coating on both sides. It is easy to use and can be applied
This shows that the Raleigh effect is negligible in the visible light on an industrial scale. However, it results in significant material waste
range. However, when light passes through a surface with roughness and requires very high coating concentrations to effective immersions.
comparable to or greater than the wavelength, the diffusion of Mie in­ The spray-coating technique is the most common technique used in
tervenes instead of Raleigh [116]. The theory of Mie is expressed by: industries. It consists of spraying the coatings on the substrates followed
by drying (Fig. 4- c) because of its efficiency. However, it may result in
( / ) ∑
∞
non-uniform thicknesses and requires several parameters to be
CSCA = π d2 2 (2m + 1) (am + bm ) (3)
m=1 controlled compared to other deposition techniques.
These three techniques are widely used for the fabrication of ori­
The parameters am and bm correspond to the magnetic and electric
ented transparent superhydrophobic coatings for optical and solar en­
multipoles of order m, respectively. According to this equation, it can be
ergy applications.
seen that the CSCA is proportional to the square of the diameter, which
implies the existence of a maximum beyond which the surface rough­
5.1.1. Suspension of nanoparticles with polymers
ness, while maintaining a superhydrophobic character, can reduce the
Qiang Li et al. [119] In a study by Qiang Li et al. [119], a
transparency by generating light scattering. Therefore, manufacturing a
self-cleaning, transparent, and durable coating was developed using the
transparent superhydrophobic coating requires finding the critical point
spray technique on a borosilicate glass substrate to repel and reduce dust
where the roughness high enough to ensure superhydrophobicity but
adhesion. The coating was based on SiO2 nanoparticles and a silicone
optimized for transparency. On an experimental side Yudi Rahmawan
resin, crosslinked using UV. The coating showed excellent super­
et al. [117] measured total Mie diffusion as a function of different par­
hydrophobicity and very good transparency of up to 80%. Abrasion
ticle sizes. The results showed that particle diameter leads to an expo­
tests, impact of droplets, and boiling of hot water were carried out on the
nential increase in total Mie scattering.
coating, and the results were very good. Chuan Zhang et al. [120] pre­
Consequently, a surface roughness lower than the wavelength of
pared a superhydrophobic coating using the spray-coating method and
light can significantly reduce the Mie effect. According to research, a
hydrophobic SiO2 nanoparticles of 10 nm size with a non-fluorinated
surface roughness of less than 100 nm (less than λ/4 of visible light) may
resin. The coating had a contact angle of 160◦ with a low sliding
be the sweet spot for making a highly transparent superhydrophobic
angle, generating an excellent self-cleaning character. It was found that
surface in visible light. In this sense, it has been demonstrated in several
the transmittance of the coating strongly depends on the resin/­
works the fabrication of transparent and superhydrophobic coatings
nanoparticle ratio, and the coating showed a transmittance of 91.03% in
simultaneously is successful [118], but the nanostructure required for
the visible range. Zihui liang et al. [121] fabricated a transparent
superhydrophobicity is generally vulnerable to mechanical tests. This
superhydrophobic coating using SiO2 modified by trimethox­
vulnerability creates a contradiction between superhydrophobicity,
ypropylsilane (PTMS) and PDMS resin. The SiO2/PDMS nanocomposite
transparency, and durability, which is among the major obstacles in this
suspension was deposited on a glass substrate via the spin-coating
field.
method (Fig. 5). The coating exhibited a contact angle of 158◦ with
80% greater transparency. The addition of PDMS played an important
5. Manufacturing of transparent superhydrophobic surfaces role in improving the thermal resistance of the coatings. Additionally,
heat treatments were applied to the surface, and the coating showed
Roughness and surface composition are two main parameters in the good stability from − 15◦ up to 450 ◦ C without loss of
development of superhydrophobic and transparent coatings. Through superhydrophobicity.
technological advancement, several deposition methods have been In another Work, Mahendra S. Kavale et al. [122] prepared a trans­
developed and can generally be categorized in two groups: methodical parent superhydrophobic glass by depositing a coating using the
top-down approaches and bottom-up approaches. Top-down approaches dip-coating method. They used Polymethyl methacrylate (PMMA) and a
are used to create ordered surfaces based on treatments such plasma silica sol prepared from the metallic precursors of Trimethox­
treatments, acid etching and laser etching. Bottom-up approaches, on ymethylsilane (MTMS). The MTMS was mixed with water and Ammo­
the other hand, are used to produce arbitrary surfaces and include nium fluoride (NH4F) in ethanol leading to a reaction of hydrolysis and
techniques such as electrospinning, layer by layer, self-assembly, sol-gel condensation. The hydrolyzed MTMS was then reacted with polymethyl
methods. methacrylate (PMMA), which modified the hydroxyl groups of the sur­
This section aims to describe and highlight the progress made so far face by CH3 groups, generating hydrophobic nanoparticles. The study
in the manufacturing of transparent superhydrophobic coatings for use examinated the variation in PMMA concentration from 1% to 8% and
in solar energy applications. the results showed that the increase in the concentration of PMMA lead
to the increase in the contact angle. The coating showed a maximum
5.1. Solution processing techniques contact angle of 171◦ for a concentration of 7%, while for the same
concentration, the coating showed 91% transparency. Sangeetha Sriram
Coating deposition techniques are the most widely used techniques et al. [123] used the same deposition technique.to created a transparent
for preparing thin layers under ambient conditions, However, these superhydrophobic glass using a combination of PMMA and SiO2 nano­
techniques require the use of a solvent, which means they cannot be particles. In the experimental protocol, PMMA and SiO2 are dispersed in
used for insoluble and crosslinked polymers. The deposition process toluene, and perfluorooctyl trichlorosilane (PFOTS) was added to the
generally consist of two steps: a deposition step followed by a drying reaction. The obtained suspension was applied by dip-coating on a glass
step to remove solvent and change the physico-chemical properties of substrate, forming a layer with a thickness of 6.60 μm. The coating
the surface. increased the contact angle from 32◦ to 174◦ , with a slip angle of 2◦ ,
The spin coating technique is a very simple method that involve which providing self-cleaning character to the glass surface (Fig. 6). The
depositing a coating suspension onto a using centrifugal force at high coating showed a transparency of 85%, with a decrease of 9% compared

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

Fig. 4. Principle of deposition techniques by: a) Spin-coating b) Dip-coating c) Spray-coating.

Fig. 5. Schematic illustration of the manufacturing process of a superhydrophobic SiO2/PDMS coating via the spin-coating method [121].

Fig. 6. Images are showing the self-cleaning property on the uncoated and coated glass surface, where the water droplet collected the dirt along with it while rolling
down from the surface. Whereas such a phenomenon not seen on the uncoated surface [123].

to the uncoated glass substrate (Fig. 7-b). Additionally, due to the superhydrophobicity or change in surface morphology.
presence of silica nanoparticles that are chemically inert, the coating Another very simple method has been proposed by Wang et al. [124]
exhibited thermal stability up to 380 ◦ C without losing super­ produced a superhydrophobic coating based on PU-PMMA and fluori­
hydrophobicity (Fig. 7-a). The coating also showed very good stability nated SiO2 nanoparticles using the spray-coating method. The
against different solvents of various pH, even after immersion for 400 h. PU-PMMA colloids allowed the formation of an interpenetrating
UV ray tests were also applied to the coated glass, and the results showed network in to properly stabilize the SiO2 nanoparticles. This resulted in a
that the coating exhibited excellent UV ray stability without any loss of hierarchical surface morphology and very low surface energy due to the

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

Fig. 7. a) Water static contact angle of the coating after 1 h annealing at different temperatures. b) UV–Vis spectrum of uncoated and coated glass trans­
mittance [123].

presence of fluorine molecules. The combination of these two conditions Not only SiO2 nanoparticles are used for the preparation of super­
increased the contact angle up to 165◦ with a very weak slip angle. The hydrophobic coatings. For example Amrita Hooda et al. [126] manu­
coating showed very good stability to chemical solvents and UV rays, factured a superhydrophobic coating using a combination of ZnO and
with very good abrasion resistance up to 200 cycles without losing Polystyrene through the spin-coating method. First, the ZnO nano­
superhydrophobicity. The optical properties of the coating were also particles were functionalized by chlorotrimethylsilane and 3-mercapto­
identified, and the results of transmission showed 80%. propyltrimethoxysilane. After the double functionalization of the
In another paper, Amrita Hooda et al. [125] reported a simple nanoparticles, they were mixed with the polystyrene resin, and then the
method for the fabrication of a highly transparent superhydrophobic final suspension was applied to a glass substrate by the spin-coating
glass using a polystyrene resin in combination with the SiO2 nano­ method. The effect of varying the concentration of nanoparticles from
particles. First, the SiO2 nanoparticles were functionalized by Trie­ 1% up to 25% on the contact angle was examined. The results showed
thoxyoctylsilane (TOS) through a hydrothermal reaction. Then, they that increasing the concentration from 1% up to 20% led to a significant
were mixed with the polystyrene resin, the final suspension was applied increase in surface roughness and consequently an increase in contact
to a glass substrate by the dip-coating method. The coating showed a angle. The coating exhibited a contact angle of 152◦ and a slip angle of
porous hierarchical morphology exhibiting V-form dyads to trap the air 3◦ at 20% concentration. Moreover, despite the deposit of the coating,
between the surface nanostructure, generating a nanoscale roughness of the transparency of the glass is not impacted compared to the uncoated
84.96 nm. Superhydrophobicity and transparency were taken into ac­ glass (Fig. 9), The coated surface presented a transmittance between
count depending on the variation of dipping and pulling speed in the 89.9% and 91.9% in the visible range (Fig. 9).
dip-coating process. The coating showed a contact angle of 162◦ and a Zhang et al. [127] created a superhydrophobic glass surface using a
low slip angle of 3◦ , The coating application resulted in highly trans­ coating based on carbon nanotubes and PDMS as a source of silica.
parent surfaces with a transmittance of 91.8%, almost no impact on the Firstly, the carbon nanotubes are functionalized by octadecylamine and
transparency of uncoated glasses which exhibited a transmittance of then dispersed in PDMS. The resulting dispersion was deposited on a
92.6% (Fig. 8). glass substrate by the spray-coating method and then calcined at a high

Fig. 8. The percentage of transmission as a function of wavelength for bare Fig. 9. The percentage of transmission as a function of wavelength for bare
glass and glass coated with PS/SiO2 nanocomposites120. glass and glass coated with PS/ZnO-20 nanocomposites [126].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

temperature of 550 ◦ C to obtain a transparent surface with hydrophilic

nanotubes. To further reduce the surface energy, PDMS was deposited
using he chemical vapor deposition (CVD) method. The surface exhibi­
ted a contact angle of 165◦ with a slip angle of 3◦ . The surface also
exhibited interesting optical properties with a transmittance of 83%.
The coated glass was applied to solar panels to study its performance,
and the results showed that the current-voltage curves for the coated and
uncoated substrates were almost identical (Fig. 10). This indicates that
the application of this coating does not impact the performance of the
panels, but on the other hand provides a self-cleaning character capable
of repelling contamination easily, which can improve the performance
of the panels.
Likewise Allahdini et al. [128] developed a hyper-transparent
superhydrophobic coating with a transmission of 80% by the
Fig. 11. The effect of superhydrophobic coating on the reduction of dust on the
spray-coating method. They used SiO2 nanoparticles, an alkoxysilane
surface of glasses: on the left surface of uncoated glass, on the right surface of
binder, and methyltriethoxysilane as a coupling agent between the bond
coated glass [130].
and the nanoparticles to improve the stability of the coating. The coating
showed a contact angle of 163◦ with a low slip angle and interesting
resins for the manufacture of transparent superhydrophobic coatings,
durability.
other resins have shown their effectiveness in the preparation of this
Elbruz Murat Baba et al. [129] prepared a superhydrophobic nano­
type of coating. For example Zhongfen Ji et al. [131] prepared a
composite coating using hydrophobic nanoparticles and polystyrene
self-cleaning hybrid superhydrophobic coating using the resin of SiO2
resin via the spin-coating method. Firstly, hydrophobic SiO2 nano­
nanoparticles modified by Perfluorodecyltrimethoxysilane (PFTS) with
particles were dispersed in toluene, and then the PS resin was added to
the resin of GPDF containing epoxy groups and fluorinated chains. They
the suspension of the nanoparticles. The final product was applied on the
used the technique of spin-coating and studied the effect of the variation
glass substrate using the centrifugation method. The increase in the
of GPDF ratios compared to the concentration of nanoparticles on the
surface concentration led to an increase in roughness and contact angle.
surface wettability. It was observed that the contact angle increases with
The coating showed a maximum contact angle of 172◦ ; however, it was
the increase in the ratio of GPDF/SiO2. The coating showed a contact
noticed that transparency decreased with an increase in the concentra­
angle of 160◦ with a low slip angle, enabling the surface to have a
tion of nanoparticles. It was concluded that the point of balance ensuring
self-cleaning superhydrophobic character capable of removing dust
minimum light scattering while maintaining superhydrophobicity was
easily with a few drops of water (Fig. 12). The coating showed a very
at an 80% concentration of nanoparticles.
high transmittance up to 93.6%. Moreover, the coating has shown good
Also, Li-zhi Zhang et al. [130] prepared a superhydrophobic coating
stability towards solvents of different pH, it was able to maintain
based on SiO2 nanoparticles and organic silicon resin. The coating
superhydrophobicity at high temperatures up to 200 ◦ C (Fig. 13-b-c),
exhibited a contact angle of 153◦ and a slip angle of 9◦ . The study found
and at UV exposure up to 7 days with almost no impact (Fig. 13-a). Even
that the coating deposition reduced the number of dust particles
in the mechanical peeling tests, the coating retained a contact angle of
deposited on the surface compared to an uncoated surface, even at
up to 140◦ after 200 cycles.
different angles of inclination. This was due to the low adhesion energy,
which allowed the particles to slide easily on the surface by the force of
gravity (Fig. 11). Furthermore, the study observed that the deposition of
the coating improved the transmittance of the glass for wavelengths of
400 nm–800 nm. The coating exhibited a transmittance of 91.4%, which
was attributed to its ability to reduce spectral reflectivity. This
improvement in transmittance was observed even after dust deposition
tests with different inclination angles of 30◦ , 45◦ , and 60◦ .
Moreover, in addition to PDMS, PMMA and PS, which are classic

Fig. 10. Current-voltage curve of monocrystalline silicon solar cells prepared Fig. 12. The effect of the coating on the self-cleaning property: (a) the original,
on a coated glass substrate with or without coating [127]. (b–c) the process and (d) the final state [131].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

Fig. 13. (a) Various CA of the UV-exposed over 7 days. The CA of the coated surface (b) before and (c) after the thermal treatment [131].

In similar work Shuangjie Zhao et al. [132] proposed an additive 150◦ and very high optical properties. In a more advanced study, Yujin
coating process for manufacturing transparent superhydrophobic glass Lee et al. [133] proposed a simple approach for fabricating a transparent
using polyfurfuryl alcohol (PFA) and silica species deposited by the superhydrophobic surface with controlled roughness using a
spray coating method. The coated glass substrate was annealed at high double-scale nanostructure. They prepared a suspension of 50 nm Al2O3
temperature to remove PFA nanoparticles. The effect of varying the nanoparticles in 2-propanol and added Al2O3 nanoparticles of 20 nm
PFA/SiO2 ratio from 0.5 to 2.5 was studied. Fig. 14 summarizes the size to the suspension at varying weight percentages. The heterogeneous
obtained results. It was observed that increasing the PFA/SiO2 ratio mixture was then applied to a glass substrate using the spin-coating
significantly lead to an increase in the contact angle up to 170◦ method and dried at 150 ◦ C. Next, an aluminum nitrate solution was
(Fig. 14-a). However, increasing this ratio lead to a decrease in trans­ deposited on the same layer of nanoparticles to improve the stability of
parency from 90% to 70% (Fig. 14 – b-c). At the equilibrium point, the the adhesion between the nanoparticles. The substrate was then dried at
coating showed a contact angle of 162.2◦ with a transmittance of 86%. 150 ◦ C and immersed in a solution of octadecylphosphonic acid for
Additionally, the coating’s performance was tested by its outdoor surface hydrophobization, followed by drying. The use of double-scale
exposure, and it was graded as hydrophobic with a contact angle of 154◦ particles allowed for the creation of a rough surface with pores to trap
even after 90 days of exposure. air. Increasing the weight percentage of the 20 nm Al2O3 nanoparticles
led to the formation of micropapillae, which increased the surface
5.1.2. Suspension of nanoparticles without polymeric resin roughness and, consequently, the contact angle. The resulting surface
Xu et al. [93] prepared a transparent superhydrophobic coating showed a contact angle of 161◦ , a slip angle of less than 2◦ , and a
based on 100 nm silica nanoparticles modified with fluorosilane using transmission of 91%. It also exhibited excellent self-cleaning properties
the spin-coating method. The coating was prepared using a mass con­ (Fig. 15-a), . When a quantity of dust was deposited on the surface, the
centration of 0.8%. The resulting coating exhibited a contact angle of transparency was reduced up to 50%. However, a simple cleaning with

Fig. 14. (a) contact angle and (b) transmittance of samples with various PFA/silica volume ratios in the ink mixture Samples with volume ratios of 0.5, 1, 1.5, 2 and
2.5 are named F1, F2, F3, F4, and F5, respectively. (c) Photographs of F1, F2, F3, F4 and F5 with different water solution droplets such as fountain pen ink (blue),
milk (white), coffee (brown) and juice (yellow) [132].

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Fig. 15. The self-cleaning ability of optimized non-wetting films, (a) Photographs of self-cleaning test with bare and coated glass before (blue line) and after (red
line) self-cleaning. (b) Optical transmission of coated films before self-cleaning wi thout carbon dust (black line), before self-cleaning with carbon dust (blue line),
and after self-cleaning (red line) [133].

drops of water enabled the entire surface to be cleaned and the initial phase separation process, while the second step is to use hydrophobic
transmission to be recovered, demonstrating the effectiveness of the SiO2 nanoparticles functionalized by HMDS to reduce the surface en­
surface’s self-cleaning properties (Fig. 15-b). ergy. the resulting coating increased the transmittance of the glass
Sanjay S. latthe et al. [25] prepared a superhydrophobic coating for substrate, the deposition of the first layer increased the transmittance
solar panels by dispersing hydrophobic SiO2 nanoparticles in hexane. from 90% up to 93%, due to the presence of a nanoporous structure that
The coating was then applied directly onto the solar panels using the can trap incident light between the pores, and with the deposition of the
spray-coating method for up to 12 layers. The surface of the panels nanoparticle layer, this led to a decrease in roughness, which leads to an
showed a contact angle greater than 150◦ and a low slip angle. The increase in transmittance of up to 97.9%. Moreover, the coating showed
coating made the surface of the self-cleaning panels capable of repelling a contact angle of 157.9◦ , with a low sliding angle which provided the
contaminants with only a small amount of water (Fig. 16). surface with a self-cleaning character. It has also been observed that the
In a another work [134], a superhydrophobic and transparent coating can come into contact with acids/bases of different pH without
coating for solar energy applications prepared, by the spray-coating losing its superhydrophobicity, which can be very demanding for solar
process, using a suspension of hydrophobic silica nanoparticles in the cell applications. Moreover, it should be noted that the preparation of
presence of isopropyl alcohol (IPA) with parachlorobenzotrifluoride anti-reflective coatings can also be manufactured by the spin-coating
(PCBTF) and Cerakote as binder. The effect of the binder/nanoparticle technique. Sutha et al. [136] created a superhydrophobic glass surface
ratio on the contact angle was studied. The results showed that the based on Al2O3 nanoparticles through the spin-coating method. First an
reduction in the polymer binder generates an increase in WCA, but the Al2O3 sol was prepared and deposited on a substrate and then heat
reduction in the polymer binder also showed a reduction in the dura­ treated at 400 ◦ C for 60 min, then immersed in hot water for 20 min then
bility of the coatings. Simulated sand environmental tests were applied the surface was modified by the deposition of 1H, 1H, 2H, 2H – per­
to the coatings and the results showed that for an equivalent 10-year fluorooctyltrichlorosilane by spin-coating, then annealed at 180 ◦ C. for
sand exposure, the WCA of the surface decreased from 166◦ to 157◦ . 30 min to obtain low energy surfaces. A study of the number of layers
on the other hand, the dip-coating technique has also shown high effi­ from 1 to 4 layers was studied, the contact angle was increased with the
ciency for the preparation of superhydrophobic coatings. Jinghui Zhi number of layers up to 3 layers, then was reduced, the coating showed a
et al. [135] prepared a two-step superhydrophobic coating on the glass maximum contact angle of 161◦ , moreover the deposition of 3 layers of
of the solar cells using the dip-coating method. In fact, two solutions coating permit to increase the transmittance of the substrate from 93%
were prepared separately, for first glycidoxypropyltriméthoxysilane was to 95%. The coated substrate was applied to a solar panel, it was
mixed with ethanol, then water and octadecylamine (ODA) were added observed that the coated substrate increased the efficiency of the un­
to the solution with the use of Poly(ethylene glycol) as a blowing agent, derlying solar cell increased to 1.4% compared to the uncoated sub­
and for the second solution prepared hydrophobic SiO2 nanoparticles by strate, the deposition of dust on both substrates led to the decrease in the
the sol-gel method and functionalized by hexamethyldisilazane efficiency of the panels, after however simple cleaning, the coated glass
(HMDS), then the glass substrate was immersed in the first solution then recovered the initial efficiency of the panels up to 91% due to the
calcined in an oven, then immersed again in the second solution fol­ self-cleaning effect of the surface unlike uncoated glass could not
lowed by drying. The first step is to form a nanoporous structure by a recover the initial efficiency because of the still presence of dust

Fig. 16. The effect of self-cleaning of the coating of laying on solar panels23.

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

Table 2 containing a high active chemical component by a solution, operating at

Photovoltaic properties of a solar cell covered with uncoated and 3 layer low temperature, no expensive equipment and consumes less energy. it
aluminum oxide coated glass substrates under different conditions (as manu­ is a cost-effective, fast, easy and commercially acceptable technique
factured, under dust and after cleaning) [136]. [138]. It is one of the preferred methods to manufacture good quality
Voc (V) Isc Maximum FF η (%) superhydrophobic surfaces with thicknesses of a few micrometers, the
(mA) power (mW) thickness and morphology of the obtained surface by this technique can
Standard solar 2± 100 150 ± 5 0.7 ± 1.5 ± be easily adjusted according to the components and the protocols [139].
cell 0.15 ±5 0.05 0.05 The sol-gel technique has shown very good success in the preparation of
Uncoated 2.12 ± 103 121 ± 4 0.56 ± 1.2 ± superhydrophobic coatings and especially superhydrophobic coatings
substrate 0.02 ±2 0.045 0.05
as – Fabricated B3 2.15 ± 103 139 ± 5 0.63 ± 1.4 ±
which require high transmittance, generally, sol-gel method is assisted
substrate 0.01 ±1 0.003 0.02 by three ways (spin-coating, dip-coating, spray-coating) are often the
Uncoated 2.05 ± 43 ± 51 ± 4 0.58 ± 0.51 ± most used for the manufacturing of self-cleaning surfaces. Zhang et al.
substrate Under 0.01 4 0.01 0.02 [140] reported a simple method for the fabrication of a super­
dust
hydrophobic coating by the sol-gel method, the coating showed a con­
B3 under dust 2.07 ± 59 ± 71 ± 7 0.58 ± 0.71 ±
0.011 2 0.011 0.009 tact angle of 154◦ and a transmission of 93.5%, with a loss of 6.5%
Uncoated 2.09 ± 68 ± 86 ± 4 0.6 ± 0.86 ± compared to the uncoated surface. Chong Ke et al. [141] made a
substrate after 0.02 3 0.005 0.05 transparent superhydrophobic coating also by the sol-gel method with a
cleaning transmittance lower than 1% compared to the bare surface, first they
B3 after cleaning 2.21 ± 100 123 ± 9 0.56 ± 1.23 ±
prepared a sol of Si(OH)4 then they were mixed with nanoparticles of
0.01 ±2 0.001 0.015
SiO2 dispersed in ethanol, then the coating was poured onto the glass
B3: The surface coated with 3 layers of superhydrophobic coating. substrate, the coated substrate was dried at 80 ◦ C and then heat treated
at 550 ◦ C for 4 h in order to improve the mechanical properties, and
(Table 2). finally the substrates were immersed in a perfluorooctyl trichlorosilane
in the similar work, Wei Li et al. [137] manufactured a super­ (PFOTS) solution for 1 min to decrease the surface energy. The effect of
hydrophobic and anti-reflective coating, using SiO2 nanoparticles, using varying the amount of SiO2 nanoparticles on the surface wettability was
the Spin-coating technique. First SiO2 nanoparticles were made by the studied, the results showed that increasing the amount of nanoparticles
sol-gel method, the silica sol was deposited a glass substrate by spin leads to an increase in the contact angle, from 1 g of nano SiO2 the
coating, then dried and calcined at high temperature, then the sol of coating presented a superhydrophobic character, the maximum value
hexadecyltrimethoxysilane (HDTMS) was also deposited by the same obtained was 154◦ , on the other hand by the effect of the sol Si(OH)4 was
deposition technique, followed by drying. The coating exhibited porous also studied, it was observed that the increase in the amount of Si(OH)4
hierarchical morphology, with a thickness of 146 nm, in addition the negatively influences the transparency. The coating showed a
coating not only kept the transparency of the glass substrate but also self-cleaning character, with high thermal stability up to 200 ◦ C without
increased the substrate transparency, the coating exhibited a trans­ loss of superhydrophobicity. In another work, Czyzyk et al. [142]
mittance of 99%. at 580 nm (Fig. 17-a). The number of layers by spin developed a transparent superhydrophobic coating by the sol-gel
coating was studied, the results showed that the deposition of two layers method, using silica NPs with metal precursors of 3-glycidyloxypropyl­
which presented the highest transmittance and contact angle up to 147◦ , trimethoxysilane, Vinyltrimethoxysilane, and Dynasylan F-8263, the
with a slip angle of less than 10◦ , which gives it a self-cleaning character. coating was applied to a glass substrate by spraying. They used tem­
The coating was applied to photovoltaic cells, and the application of the perature curing, UV curing, or both, to test the effect of the curing step
coating was found to improve cell performance, increasing current on surface properties. It has been found that the use of double cures has
density by 6.78% (Fig. 17-b), and improving energy conversion effi­ allowed to obtain a coating much stable and more resistant to me­
ciency by 10.12%. chanical tests and to the test of UV rays due to the higher degree of
condensation reactions, compared to the use of only one. average
5.2. Sol-gel method hardening, the coating was able to keep a contact angle greater than
150◦ even after exposure to UV rays for 1000 h (Fig. 18). Plus
The sol-gel technique is a method of processing a compound

Fig. 17. a) UV transmission spectra against silica nanoparticles coated with glass, bare glass, and their difference. b) comparison of the current density of photo­
voltaic cells with coated and uncoated glass [137].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

entire surface. And finally, the coated substrate was dried at 80 ◦ C for 2 h
and then 1 h at a temperature of 120 ◦ C. the coating deposited was
103.54 nm thick, exhibits a hierarchical morphology, with a nanoscale
roughness of 3.48 nm, the coating exhibited a contact angle of 162◦ with
a slip angle of 1.5◦ , in addition the coating exhibited a 95.5% trans­
mittance with a 5% increase over uncoated surface. Mechanical pencil
hardness tests were applied to the coating and the results showed that
the coating showed very good resistance to the 1B pencil test and 2B
pencil test, but unfortunately no resistance to the 1H pencil test.
on the other hand, it is still possible to prepare the self-cleaning
coatings by the sol-gel method without the need to use the nano­
particles to create a rough surface. Pratiwi et al. [145] have proposed a
simple method for the fabrication of a transparent and stable super­
hydrophobic coating using the sol-gel method, using a titanium dioxide
Fig. 18. Sliding angle versus exposure time and contact angle after 1000 h and modified substructure followed by octadecyltrichlorosilane modi­
exposure in the Q-UV test for all three curing processes136. fication, in fact in first a solution of peroxotitanium complex was pre­
pared, then a glass substrate was immersed in this solution for 30s
followed by drying, the coated glass was placed in a solution of octa­
superhydrophobicity, the coating showed 90% transmittance.
decyltrichlorosilane (OTS) for 6 h followed by drying for 3 h (Fig. 19).
Moreover, the sol-gel method is not only used to prepare super­
The coating showed a contact angle of 158◦ with a slip angle of 4◦ , which
hydrophobic and highly transparent coatings, but it is also used to
gave better self-cleaning efficiency (Fig. 20). the coating has shown very
prepare coatings which improve the transparency of surfaces. Rubing Xi
good chemical stability which can withstand for days in solution of
et al. [143] prepared a mechanically stable transparent super­
different pH without loss of superhydrophobicity. In addition, the
hydrophobic nanocoating using the dipping method using hydrophobic
coating also showed very good stability to UV rays up to 300 min.
silica nanoparticles and highly cross-linked silica sols as an inorganic
In the similar work, Satish A. Mahadikun et al. [146] fabricated a
binder. The study of the effect of varying the amount of silica sols was
transparent superhydrophobic coating by a simple and inexpensive
studied, and the results showed that the increase in the amount of silica
sols leads to the decrease in superhydrophobicity and transparency. The approach using the sol-gel method, first Silica alcoholsol was prepared
from the methyltriethoxysilanes by the sol-gel method at room tem­
silica sol to nanoparticle ratio of 0.6/35 showed the balance ratio be­
perature, then was deposited on a glass substrate by the dipping method,
tween transparency, superhydrophobicity and mechanical stability. The
and after drying for 6 h at room temperature, the coated substrate was
coating showed a contact angle of 150.4◦ , a slip angle of less than 2◦ and
immersed in a solution of trimethylchlorosilane diluted in hexane to
a transmittance of 96.17% with a 4% increase over bare glass. In addi­
establish the functional groups on the surface. The coated substrate was
tion, the coating showed very good scratch resistance to the 3H pencil,
dried at room temperature and then was heat treated at 150 ◦ C. to
chemical stability at a deferent pH with very thermal stability up to 250◦
strengthen the bond between the silica network and the methyl groups.
without loss of superhydrophobicity. In similar work, Deepanjana Adak
It was observed that the deposition temperature plays an important role
et al. [144] a self-cleaning superhydrophobic coating has been prepared
in controlling the transparency and surface morphology and conse­
by the sol-gel method, to improve the transparency of glasses for solar
quently its wettability, the coating showed a contact angle of 154◦ and a
glass applications. In fact, they first prepared a base-catalyzed silica sol
slip angle of 9◦ and a transparency which can go up to 89%. But un­
and modified it by hexamethyldisilazane (HDMS) and it was mixed with
fortunately, the durability of the material has not been tested.
an acid-catalyzed silica sol. Subsequently, the glass substrate was
Dafna Heiman-Burstein et al. [147] created a hybrid self-cleaning
immersed in the mixed solution with a withdrawal speed of 100
superhydrophobic coating by the sol-gel method in one step, the
mm/min then the coated glass was immersed in a solution of HDMS
cleaned glass substrates were deposited in a container, the ethanol and
diluted in IPA for 2 h in order to ensure the functionalization of the
water were added to the container and then the hydroxide ammonium

Fig. 19. The procedure for manufacturing the transparent and superhydrophobic surface by sol-gel method [145].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

Fig. 20. Simulation of self-cleaning of (a–d) superhydrophobic glass and (e–h) uncoated glass [145].

until the pH of the solution becomes 10.5 and thereafter the TEO­ chemical etching method, chemical etching of the substrates by
S/alkyltrimethoxysilane, and the reaction medium was left under stir­ hydrogen fluoride at room temperature between 10 min and 25 min
ring overnight. Finally, the substrates are cleaned and dried at room followed by immersion in a sodium chloride (NaCl) solution for 3 h. The
temperature. A series of samples was prepared by varying the ratio of etched substrates, after drying, were immersed in a hexane solution
TEOS/alkyltrimethoxysilane between 9:1 and 1:9. Different alkyl­ containing 10 mmol of trichloro (1H,1H,2H,2H-perfluorooctyl) silane
trimethoxysilane were used such as vinyltrimethoxysilane, propyl tri­ for 10 min, followed by drying at 100 ◦ C. the effect of HF etching time on
methoxysilane, isobutyl trimethoxy silane, octadecyltrimethoxysilane, the wettability was studied, the results showed that the increase in
decyltrimethoxysilane, phenyl trimethoxysilane, however only for etching time leads to the increase in contact angle, the surface showed a
octadecyltrimethoxysilane and decyltrimethoxysilane the super­ maximum contact angle of 164◦ with a slip angle of 5◦ , and after the
hydrophobic surface was obtained. this was explained by the effect of surface was immersed in the NaCl solution, the surface roughness
the substituents and the length of the allylic chains, it was found when changed from micrometric roughness to nanometric roughness, and
the length of the chains is insufficient, the condensation of thereafter consequently the increase in the contact angle up to 168◦ . The coating
(TEOS) and alkyltrimethoxysilane takes place simultaneously which showed very interesting durability during one month storage in air and
prevents the formation of a nanoparticle (see Fig. 21-a), on the contrary water with almost no loss of contact angle. Also Phuong Nguyen-Tri
when the chain length was increased to Octadecyltrimethoxysilane et al. [151] prepared a superhydrophobic coating based on tetraethyl
(ODTMS) or decyltrimethoxysilane (DTMS) it was observed the forma­ orthosilicate silica (TEOS) nanoparticles via the dip-coating method
tion of nanoparticles and consequently a rough superhydrophobic hi­ using chemical etching with Sodium hydroxide (NaOH) and plasma
erarchical surface (see Fig. 21-b-c). etching, according to Table 3 it was noticed that the treatment chemical
The sol-gel method remains one of the most effective methods for by NaOH has increased the contact angle from 91◦ to 147◦ , which shows
inorganic materials, has several advantages, it often presents coatings the importance of chemical etching in improving the super­
with good heat resistance, very good mechanical stability, and excellent hydrophobicity of the surface, on the other hand it was also noticed that
anti-wetting properties, and above all it allows to easily form porous increasing the concentration of nanoparticles leads to an increase in
nanostructures under specific reaction conditions, however it is a pro­ roughness, causing the creation of nanostructures on the surface and
cess that generates chemical pollution, and it takes a lot of time. consequently increasing the contact angle up to 160◦ , and increasing the
TEOS concentration also has the same effect on the contact angle as
5.3. Etching method increasing nanoparticles. In addition, plasma etching also showed
similar efficiency as chemical etching, the surface showed a contact
Etching is one of the most accessible methods for self-cleaning sur­ angle of 173◦ . The surface prepared either by chemical etching or by
face preparation, including photolithography, wet chemical etching and plasma etching showed very good stability in abrasion tests, the results
plasma etching. Meng Xu et al. [149] prepared a superhydrophobic showed that the surface retains its superhydrophobic character even
surface by chemical etching, the surface exhibited a contact angle of after 30 cycles.
152.7◦ with a low slip angle. In addition, the surface prepared by this In another work, Wenqing Hou et al. [152] proposed a simple
chemical etching method showed good stability in mechanical tests of method for the preparation of self-cleaning superhydrophobic coatings
4H pencil hardness test. In another work, Jae-Hun Kim et al. [150] using plasma etching method. In the experiment, a substrate was
fabricated a self-cleaning superhydrophobic coating by the two-step cleaned and then covered with SU-8 silica resin with a photoresist, then

Fig. 21. SEM images of coatings composed of a) TEOS: alkyltrimethoxysilane, (b) TEOS:DTMS, and (c) TEOS:ODTMS at a molar ratio of 5:5 [147].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

Table 3 the coating showed good transparency, but it was observed that after the
Processing conditions for the fabrication of superhydrophobic fabrics by pro­ plasma step the substrate loses some transparency compared to the bare
cedures without etching step (a) and with etching step (b− f) [151]. surface a cause of the modification of the visible changes.
Samples Pretreatment Solution A step 1 Solution B Contact Park Joonsik et al. [153] fabricated a superhydrophobic coating by a
step 2 angle (deg) simple method using colloidal lithography with ion etching. The poly­
a Water/ SiO2 (8%) + water TEOS 91 ± 1 styrene manospheres of size 100 nm were diluted in methanol and
ethanol (300 mL) + acetic acid (10%) Triton, a single layer of the manospheres were deposited on the glass
(2 mL) substrate by spin-coating, then the monolayer of the manospheres were
b NaOH (0.5 SiO2 (8%) TEOS 147 ± 1
etched by plasma and then were chemically treated by (tridecafluoro-1,
M) (10%)
c NaOH (0.5 SiO2 (10%) TEOS 152 ± 1 1,2,2-tetra-hydrooctyltrichlorosilane to decrease the surface energy
M) (10%) using the vapor deposition method. The effect of varying the rotational
d NaOH (0.5 SiO2 (12%) TEOS 160 ± 2 speed of spin-coating relative to the deposition of the polystyrene
M) (10%) monolayer was studied, the results showed that the speed 4000 rpm was
e NaOH (0.5 SiO2 (12%) TEOS 173 ± 2
M) (15%)a
the most approximate most optimal speed to form the lowest network
f plasma SiO2 (12%) TEOS 173 ± 2 density with the highest contact angle. With this speed the surface
(15%)a presents larger micro-voids compared to the other speeds tested. And
g Plasma SiO2 (12%) 2 wt % of TEOS 167 ± 2 after having been etched for 20 min the surface presented nanopillars
acrylic resin (15%)a
with a height of 450 nm consequently forming a nano o hierarchical
a
Exceptionally, solution B was prepared in benzene instead of toluene. structure provides a superhydrophobic character to the surface.
The etching technique has shown some advantages in the prepara­
a model mask was deposited on the surface, then the assembly was tion of highly transparent self-cleaning superhydrophobic coatings with
exposed to UV for 10s. the substrates are treated by plasma etching to high mechanical properties, however it is a relatively expensive process
etch the surface and finally generate a surface with micro-cubics, finally and requires high precision.
the treated substrates are chemically modified by Heptadecafluoro-1,1,
2,2-tetrahydrodecyl triméthoxysilane (FAS) followed by drying. Ac­ 5.4. Impression by lithography
cording to the SEM results, the surface showed a cubic nanostructure
with side lengths of 20 μm, distributed evenly on the surface without This method can also be used to generate self-cleaning hierarchical
defect, with a variation of the spacing distance between the centers of surfaces. It allows for the precise control of surface morphology based on
the cubes between 30 μm. and 130 μm, it was observed the spacing the replication of master information. The lithography technique can be
distance has a direct effect on the contact angle, increasing the distance classified into several classes depending on the types of substrate and the
from 30 μm to 60 μm leads to an increase in the value of the contact source of power used (X-ray, UV, electron beam, etc.). However, like
angle up to ‘on presentation of the value of the maximum contact angle most techniques, each class of lithography has certain advantages and
of 154.22◦ at 60 μm then between 60 μm and 100 μm the contact angle disadvantages.
begins to decrease to 148◦ and from 100 μm the value of the contact Yoon et al. [154] prepared a wet-style transparent superhydrophobic
angle the value of the contact angle gradually decreased to 118◦ due to coating that provides superhydrophobicity and prevents fogging even in
the passage from the cassie-baxter state to the Wenzel state. Yongxin humid environments. The design of this coating was carried out using
Wang et al. [148] created a superhydrophobic and transparent poly lithography techniques. Initially, PDMS was glued onto a surface con­
(ethylene terephthalate) surface using a combination of dip-coating, taining micropillars, and then demolded to create a negative structure
plasma treatment and the CVD technique, first the Polyethylene tere­ on the PDMS polymer. The pores were filled with a photocurable ma­
phthalate (PET) substrates are immersed in a binder solution based on terial, and this loaded PDMS polymer was fixed onto a polymer-silica
methylphenyl silicone by monitoring the deposition of hydrophobic composite. Subsequently, the surface was UV treated to transfer the
SiO2 nanoparticles then the substrates are treated with O2 plasma for 10 network of perfluoropolyether (PFPE) pillars onto the polymer-silica
min to create hydroxyl groups on the surface to allow the formation of composite surface (see Fig. 23). The coating exhibited 90% higher
covalent bonds with perfluorotrichlorosilane which will be deposited in transmittance, a contact angle of 162◦ , a slip angle of 3◦ , and better
the second step by CVD technique (see Fig. 22). The coating deposited anti-fog performance.
was 300 nm thick, and exhibited a contact angle of 170◦ , 165◦ , 153◦ Jerome et al. [156] constructed a transparent superhydrophobic
respectively with water, ethylene, and hexadecane. the coating deposi­ surface using the Tetrafluoromethane/Argon plasma lithography and
tion improved the resistance of the PET substrate against wear, the etching method. Firstly, the silicone molds were treated with a liquid
coating retained their superhydrophobicity even after 100 cycles of phase deposition process. Then, polymeric or aluminum membranes,
wear due to the presence of the methylphenyl silicone resin. In addition, depending on the type of substrate (PET, PMMA, FEP), were used for the

Fig. 22. Schematics of chemical reactions between superhydrophobic coating and PET substrate after plasma treatment [148].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

Fig. 23. Schematic of transferring micropillar array on the polymer–silica nanocomposite using two-step lithography [154].

printing process. They were heated to a temperature below their Tg and h for the PUA curing process, and finally, the PUA film was peeled off. To
then compensated by high pressure at a printing temperature below Tf. create active OH functions on the PUA film surface, the positive u-post
Finally, the mold-polymer-membrane assembly was cooled and the PUA film was immersed in a solution of demineralized water/­
printed polymer was removed. The surface was then plasma treated to Ammonium Hydroxide/Hydrogen peroxide. The obtained film was
deposit fluorine. The combination of the two technologies enabled the washed with water and then dried with nitrogen gas. On the other hand,
production of a hierarchical surface for the three substrates, which an Si substrate was spin-coated with PDMS and deposited on a hot plate
showed a contact angle of 160◦ with a slip angle of 2◦ . Moreover, it was at 300 ◦ C. The treated u-positive PUA film was fixed below 20 mm from
found that the structure of the roughness and its inhomogeneity, the the PDMS heated, and after the reaction, the film was removed and ul­
degree of oxidation, and the variation in the percentage of fluorine have trasonically cleaned. SEM results showed that the surface exhibited
a direct effect on the stability of the coating. In another study, Mehran u-pots of a cylindrical shape with a height of 20 μm, a circular upper
et al. [157] fabricated a superhydrophobic surface using a combination surface with a diameter of 20 μm, and a pitch distance of 80 μm. After
of lithography and spin-coating techniques inspired by the lotus leaf immersion in the solution of demineralized water/NH4OH/H2O2, the
nanostructure. Initially, a lotus leaf was cut and cleaned, and a layer of surface roughness increased progressively due to the hydrolysis reac­
PDMS was deposited on it and cured at room temperature for three days. tion, which led to the oxidation of the surface. However, after the
The film was then peeled off to obtain a negative structure of the lotus deposition of a layer of PDMS, the surface roughness decreased. The
leaf nanostructure on the PDMS film, which was subsequently used as a obtained maximum contact angle was 146◦ . Moreover, the super­
model to fill the microcavities with a solution of starch, poly­ hydrophobic PUA film can maintain its high contact angle even after 50
hydroxyurethane, and cellulose nanocrystal to create a structure similar times of bending with a bending angle of 60◦ . The coating showed
to the lotus leaf. The film was then dried and removed, and a layer of excellent transparency in the visible range with 80% higher trans­
PDMS with a thickness of 2–4 μm was deposited by spin-coating, fol­ mittance. After applying the coated substrate on the solar panels, the
lowed by the deposition of a layer of silica nanoparticles functionalized solar cell showed a power conversion efficiency (PCE) of 7.95%, which
by vinyltriethoxysilane by spin-coating. Finally, the film was cured at a was very close to the bare cell’s PCE of 8.30% (see Fig. 24).
temperature of 80 ◦ C. The resulting surface showed a contact angle of The lithography process is a direct and simple approach to the
150◦ with a low slip angle, which gave it a self-cleaning character. fabrication of superhydrophobic coatings with well-controlled nano­
Mechanical tests, including knife scratches, water jet impact, finger structures. However, the impact of the intrinsic properties of light
rubbing, peeling, and abrasion, were performed on the coating, and it diffraction on the size of the patterns makes the application of this
showed good resistance to these tests. Another example by Dong et al. technique on irregular surfaces very difficult.
[158] involved the preparation of a superhydrophobic surface using a
combination of laser interface lithography and plasma etching methods.
Firstly, a Si substrate was coated with a layer of Cr to improve adhesion,
followed by a 1.4 μm layer of PR that was spun on the surface. After
drying, the surface was exposed for 1 min on a laser designed with three
beams fixed at different angles (13.5◦ , 15◦ , and 13.5◦ ), which enabled
the formation of a honeycomb mold. Then, a film of Au was deposited on
the substrate and plasma etched to form arrays of submicron pillars. It
was observed that the height of the pillars had a significant effect on the
contact angle, where an increase in structural height led to an increase in
the contact angle with water. For a height of 1.7 μm, the surface showed
an angle of 155◦ with a slip angle less than 5◦ . An in-depth study on the
parameters impacting the adhesion of the surface revealed that the ge­
ometry and orientation of the surface pillars were important parameters
to control the adhesion of the surface. Moreover, it was also found that
as the surface fraction increases, the adhesion force increases, and
consequently, the slip angle increases. Bui et al. [155] proposed a simple
and effective method for fabricating a transparent and flexible
polyurethane-acrylate (PUA) superhydrophobic surface using lithog­
raphy technique. First, a mold of PDMS with different negative u-post
was prepared by photolithography. Then, a solution of PUA was
deposited drop by drop on the mold and a transparent support film of
PET was gently deposited on the polyurethane resin to generate a thin
film of PUA. The coated PDMS mold was then exposed to UV rays for 10 Fig. 24. Current vs voltage (J–V) characteristics of the solar cell with and
without hydrophobic film coated solar cell panel [155].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

5.5. Electrospinning In a similar work, Wenjing et al. [164] elaborated a polyimide-based

nanofibrous superhydrophobic by the method of electrospinning, at first
Electrospinning is one of the most emerging and easiest methods for the polyamides acid was prepared, and then was solubilized in dime­
producing continuous polymeric fibers of nanometer or micrometer thylacetamide (DMAc), the solution was electrophiled, and the nano­
diameters. The accumulation of these fibers on a surface can create a fibrous membrane of polyamides was thermally converted to polyimide
rough morphology. This process is suitable for many types of polymers membrane by imidation. The prepared fibrous membrane was immersed
and can be performed at room temperature. It is a protrusion technique in a solution of ethanol/ammonia/dopamine/1H,1H,2H,
in which electrical bias is supplied through the protrusion nozzle and a 2H-perfluorodecanethiol water. The prepared surface showed a rough
stranded collection plate (see Fig. 25), forming polymeric ropes on the hierarchical morphology, it was observed that the added amount of
surface. Based on this, researchers recently been exploring the use of ammonia has an effect on the variation of the contact angle, for 0.4 mL
electrospinning for the preparation of self-cleaning superhydrophobic of the added ammonia the surface showed a contact angle maximum of
surfaces. 152◦ with a slip angle of 6.5◦ . it should be noted that the choice of
Mahmut et al. [160] examined the effect of lubricant addition on polymer solubilization solvent can play a very important role in con­
surface wettability properties fabricated via the electrospinning method trolling the properties of the surface prepared by the electrospinning
using a 15% concentrated solution of polyvinylidene fluoride -co-hexa­ technique. Tas et al. [165] proposed a simple method to manufacture
fluoropropen prepared in an acetone/dimethylformamide mixture. In superhydrophobic surfaces based on a copolymer of poly(vinylidene
another work, Wang et al. [161] prepared a superhydrophobic and fluoride) and hexafluoropropylene copolymer, by the technique of
transparent film based on cellulose by the technique of electrospinning, electrospinning without the need to use nanofillers, for that the copol­
first the cellulose was oxidized in order to improve the mechanical ymer was dissolved in DMAc, DMF, and a mixture of DMF with acetone
properties and the dispersibility, then was filtered by suction, the film at room temperature overnight, a series of samples were prepared by
obtained was modified chemically by grafting methyl trichlorosilane varying the mass concentration (10%, 12.5%, 15%), then the solutions
(MTCS) to replace the OH functions with long hydrophobic chains due to are loaded into a syringe for electrospinning, the assembly in detail has
the condensation of the organosilanes, subsequently a layer of polyvinyl been explained in Fig. 25, the surface morphological characterization
butyral (PVB) mixture with stannous chloride (SnCl2) was deposited by has shown that for the formulation prepared in the Ac/DMF solvent
electrospinning, and the film obtained was first immersed in a solution mixture that this either for the 12.5% or 15% concentration, the surface
of silver nitrate (AgNO3) to deposit a layer of Ag, and then was immersed showed only smooth fibers. However, for the 10% concentrations of
for 10 s in a mixed solution of d silver ammonia and glucose. The film Ac/DMF, DMAc and DMF, the surface exhibited fibers with beads due to
exhibited a contact angle of 153◦ with a slip angle of 4◦ , with high the effect of solution viscosity. For the formulation prepared in
transparency up to 81%. Chen et al. [162] created a superhydrophobic DMF-10% showed a highest contact angle up to 156◦ and a slip angle of
surface based on elastic polyurethane chromatic polydiacetylenes by the 5◦ , moreover, it was noticed that the membrane surface showed no
method of electrospinning, the 12-pentacosadiynoic acid was dissolved decomposition up to 465 ◦ C. in addition, the electrospinning is not
in DMF, then the PU was added to the solution with stirring, the mixture limited to use a polymeric solution only, but it is possible also to use a
was electrospinned on a substrate then was irradiated for to separate the polymer in combination with the nanoparticles (nanocomposite solu­
phases, and finally the coated substrate was heat treated at temperature tion). For instance, Ahmed et al. [166] used the technique of electro­
of 80 ◦ C, the analysis of the surface showed that the electrospinning of spinning for the manufacturing of a superhydrophobic nanocomposite
PU allows to obtain smooth fibers interconnected with a diameter of coating based on polystyrene and Al2O3 nanoparticles, in the experi­
1.75 μm (Fig. 26-a), however the incorporation of pentacosadiynoic ment, the Al2O3 nanoparticles were dispersed in a mixed solution of
leads to the decrease in fiber size down to 0.56 (Fig. 26-b), after UV DMAc/THF solvents, then They were added to a solution of polystyrene
irradiation some clusters appear on the fiber surface due to phase sep­ dissolved in the same mixture of solvents. The slurry was then electro­
aration (Fig. 26-c), and finally step heat treatment, the surface of the spinned onto an alumina substrate and dried overnight. The electro­
fibers has become more hierarchical because of the appearance of the spinning of the PS only showed the presence of beads with fibers with a
clusters (Fig. 26-d). The final surface showed a contact angle of 157◦ , diameter varying between 320 nm and 433 nm depending on the vari­
furthermore the surface maintained a higher contact angle even after ation of several parameters such as the percentage of PS, the flow rate
1000 stretching cycles. and the potential of the electrospinning. However, when the

Fig. 25. Schematic view of electrospinning process [159].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

Fig. 26. SEM images of a) pure PU, b) PU-pentacosadiynoic, c) After UV traitement and d) After heat treatment [163].

electrospinning was done in the presence of Al2O3 nanoparticles, it was this technique showed very high transmittance up to 94%. Durability
noticed that the nanoparticles are dispersed in a uniform manner (see tests were also carried out on the surface, and the results showed that the
Fig. 27), and that the size of the fiber diameters is greatly reduced. The coating can provide very good mechanical stability.
surface showed a contact angle of 155◦ with a slip angle of 3◦ . Jiawei Zheng et al. [168] presented a transparent and self-cleaning
It is necessary to point out that the technique of electrospinning has surface by using an inorganic, wear-resistant, and superhydrophobic
shown great interest in the manufacture of superhydrophobic coatings coating deposited using the two-step CVD method. First, a porous
based on polymers. However, it is important to take into consideration inorganic, wear-resistant film was prepared on the glass surface by
the treatment of chemical solvents to reduce pollution. This is a prom­ applying the phase separation method of an epoxy resin-silica sol. The
ising and alternative method to obtain rough microstructures; however, prepared surface showed honeycomb-shaped pores. In the second step,
the major drawback of this technique is the poor controllability of the SiO2 nanoparticles were deposited on the surface using the CVD tech­
surface. nique to create a hierarchical morphology. Finally, the super­
hydrophobic film was successfully realized after the surface
5.6. Chemical vapor deposition (CVD) modification with fluoroalkylsilane. The coating exhibited a contact
angle of 154◦ and a slip angle of 3.2◦ , with a transmission rate of 87%
Chemical Vapor phase deposition methods permit the production of Cai et al. [169] reported a simple method for the fabrication of a
aligned nanostructures with a well-controlled diameter. CVD is a well- superhydrophobic, self-cleaning coating using candle wax and methyl­
known and highly effective technique for fabricating super­ trimethoxysilane deposition by CVD, followed by high temperature
hydrophobic coatings. In this technique, gaseous substances or elements calcination at 450 ◦ C (Fig. 28). The coating showed a contact angle of
are usually deposited onto a solid substrate to fabricate non-volatile 165◦ and a slip angle of less than 3◦ , with a transmittance of 90%, in
solid coatings/films. CVD is a highly competent and frequently used addition the coating also exhibited very good thermal stability up to
method for growing a variety of nanostructures such as nanotubes, 500 ◦ C. However, when the temperature increased to 600 ◦ C, the surface
nanoparticles, nanofibers, nanocombs, nanorods, nanobeads etc. became superhydrophilic .
Xiaocheng Huang et al. [167] prepared a superhydrophobic surface In a similar work, Liu et al. [171] proposed a self-modification
with hyper-low surface energy, with networks of nanoscale cones or­ method for the preparation of a transparent superhydrophobic
dered using the CVD technique. The nanocones were created by the coating. In the experiment glass slides are immersed in the PDMS so­
nucleation of monomer nanodroplets of ethylene glycol diacrylate and lution by varying the soaking time, then they are moved horizontally on
perfluorodecyl acrylate. The surface presented a contact angle greater a candle flame to create a rough surface, then the substrates are heat
than 150◦ with a slip angle of 2◦ . Moreover, the coating prepared with treated at 550 ◦ C for 1 h, followed by cooling to room temperature to
make the surface stable, and finally a CVD process was applied to the
treated substrates for 0.5 h at a temperature of 330 ◦ C, using PDMS as
precursors of CVD, the coating showed a contact angle of 170◦ with a
slip angle of 0◦ , and a transmission of 90%. In addition, the coating
showed good thermal stability up to 475◦ without losing super­
hydrophobicity, but at 500 ◦ C the surface becomes superhydrophilic due
to oxidation of the modifying groups. However, the coatings showed an
average resistance against the solution of pH equal 3 and 11. However,
the advantageous point of this coating that even if it loses its super­
hydrophobicity at temperature 500 ◦ C or with the immersion in the
solution of pH of 3 or 11, it was noticed that the coating can recover its
initial properties again after another CVD modification treatment of the
PDMS. Hyo Jin Gwon et al. [81] reported a simple method for the
fabrication of a self-cleaning, anti-reflective glass, for organic photo­
voltaic (OPV) solar cells, by coating the glass with superhydrophobic
nanograss (SNGC), deposited by the angled vapor deposition method.
shiny, and then the surface was modified by polytetrafluoroethylene
(PTFE) to reduce the surface energy. the coating showed very high
transparency. Moreover, it was observed that the contact angle was the
Fig. 27. The SEM/EDX mapping micrographs of the as-prepared super­
contact angle increases as a function of the thickness of the NG layer, for
hydrophobic nanocomposite coatings [166].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

Fig. 28. A general scheme of the preparation of superhydrophobic transparent hollow films by the CVD method using the candle technique [169].

the deposited thickness is 750 nm of films, the coating presented a substantiated the use of titanium as a bridge to improve coating adhe­
contact angle 150◦ higher with a low sliding angle, this gave a sion on the substrate due to the hydrolysis reaction between titanium
self-cleaning character to the surface. The performance of the coating and oxide species on the glass, forming an irreversible Ti–O–Si bond. We
was tested by its application on a solar cell, it was noticed a considerable achieved surface hydrophobicity by using trimethoxyoctyldecylsilane
improvement of PCE and Jsc of an OPV cell due to the antireflection (TMODS). We deposited the coating using different concentrations of
effect. the silica precursors and deposition temperatures ranging from 200 ◦ C to
In addition, another CVD-based method, called aerosol-assisted 400 ◦ C, with deposition times ranging from 15 to 70 min. All the samples
chemical vapor deposition (AACVD), In general, the process of this manufactured by AACVD presented a contact angle greater than 150◦ .
technique is based on the use of precursors dissolved in a solvent, in the Moreover, we noticed that an increase in deposition time led to a
form of an aerosol, pushed into the CVD chamber by a flow of inert gas. decrease in transparency, which went from 90% to 20% when the
At high temperature, the solvent in the aerosol decomposes or evapo­ deposition time increased from 15 min to 60 min. On the other hand, we
rates. The vaporized precursors, before being deposited on a heated observed that decreasing the concentration of nanoparticles resulted in a
substrate, they undergo a reaction to generate a rough surface. The higher degree of transparency. We also observed the effect of tempera­
potential to fabricate a uniform, high quality film depends on controlling ture, and the results showed that 300 ◦ C was the optimum temperature
several parameters, such as, deposition time, solution concentration, gas to produce a self-cleaning superhydrophobic surface. Below this tem­
slurry, and deposition temperature. Because of the many advantages of perature, the surface did not exhibit slippage. The coating prepared by
this technique, lately the fabrication of superhydrophobic coatings by AACVD showed much better peel resistance for up to 15 cycles
vapor deposition has shown great interest. Alessia et al. [172] fabricated compared to the coatings made by spin-coating. Additionally, the
a multi-layered superhydrophobic coating on a glass substrate by coating prepared by AACVD showed good resistance to the abrasion test
aerosol-assisted chemical vapor deposition (AACVD) methods using for up to 25 cycles. Aoyun Zhuang et al. [170] prepared a self-cleaning
different functional alkoxysilanes, in fact three layers of different pre­ and highly transparent superhydrophobic glass by depositing a coating
cursors were deposited at different temperatures.: a lower layer of of PTFE-based material using the AACVD method. The surface displayed
3-methacryloxypropyltrimethoxysilane (MPS) was deposited at 450 ◦ C, a rough morphology with micro/nanostructures. The coating showed a
an intermediate layer of tetraethylorthosilicate (TEOS) was deposited at contact angle of 168◦ and a sliding angle of 1◦ , which made the surface
350 ◦ C and an upper layer of 1H, 1H, 2H, 2H per­ self-cleaning. Additionally, the coating exhibited a high transmittance of
fluorooctyltriethoxysilane (POTS) was deposited at 270 ◦ C. In order to
create a double scale roughness. The effect of the variation of deposition
time (from 5 min to 10 min) on the transparency and the super­
hydrophobicity of the surface was studied, the results showed that the
increase in deposition time from 5 min to 10 min has leads to the in­
crease in the value of the contact angle from 164.8◦ to 167.6◦ unlike the
transparency which has experienced a strong decrease which has gone
from 90% to 55%. It was found that the deposition time of 5 min rep­
resents the best combination of transparency and superhydrophobicity,
which showed a contact angle of 164.8◦ and a transmittance of 90% with
a loss of only 10% compared to the uncoated glass. Self-cleaning tests
were applied to the coating, and very good performance was obtained,
in addition the coating showed very good thermal stability up to 400 ◦ C,
and resistance to UV rays up to 72 h, without losing super­
hydrophobicity, however for the abrasion test the coating only becomes
superhydrophobic after 5 cycles. In another work, Norbert J. Janowicz
et al. [173] fabricated a superhydrophobic and transparent nano­
composite coating using APTES-functionalized mesoporous SiO2 nano­
particles and a titanium-crosslinked polydimethylsiloxane-based
organic-inorganic polymer network via the AACVD method. We
Fig. 29. The transmittance of the coating prepared by AACVD [170].

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B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

92% (Figs. 18 and 29) and good resistance to impact tests with sand 5.7. Polymerization on the surface
particles (10 g), without losing its superhydrophobicity.
Another Process, chemical vapor phase assisted by plasma (PECVD), In the 1990s, Wang and his colleagues proposed a type of controlled
which has been discovered recently, has also shown success in the radical polymerization called atom transfer radical polymerization
manufacturing of self-Cleaning and Highly Transparent Super­ (ATRP), which allows for the easy construction of C–C bonds by intro­
hdrophobic coatings for solar energy applications, Zihui Liang et al. ducing halogen atoms into the polymer matrix. This technique has
[174] fabricated a highly transparent superhydrophobic coating using a recently become a source of inspiration for researchers working on the
combination of several deposition techniques and SiO2 nanoparticles. production of superhydrophobic coatings through the polymerization of
The coating consists of three layers. First, a lower layer of SiO2 nano­ monomers by atom transfers initiated on the surface. For example, Yibin
particles with hydroxyl groups was deposited on a glass substrate using Liu et al. [176] were inspired by the microstructure of the shark to create
the PECVD method. Then, a solution of glycidoxypropyltrimethox­ a superhydrophobic surface using the ATRP technique, which involved
ysilane (KH560) was added to the surface, which permitted the forma­ using PDMS and SiO2 nanoparticles. Initially, a mixture of PDMS with
tion of a three-dimensional network at both ends. Finally, a layer of SiO2 nanoparticles was deposited on an acrylic panel template that had a
modified by HMDS was deposited using the spin coating method to form nanostructure similar to the negative shark skin nanostructure. The
a stable structure. The coating presented a contact angle of 153◦ and a surface of the nanoparticles on the surface was chemically modified by
very high self-cleaning capacity. Aminetriethoxysilane, and then immersed in a solution of α-bromoiso­
In addition, the coated substrate showed 94% transmittance with butyryl bromide. Next, poly(2-perfluorooctylethyl methacrylate)
only a 3% difference from the uncoated glass. Chemical and mechanical brushes were polymerized using ATRP polymerization in the presence of
stability tests were carried out on the coating, and the results showed Copper(I) bromide (CuBr). The authors found that the polymerization
that the surface has excellent chemical stability. It was able to maintain time and the immersion solvent had a significant effect on the contact
its superhydrophobicity even after immersion in a NaCl solution (10% angle, and the surface showed a maximum contact angle of 166◦ with a
wt) for 48 h. The coating also showed better stability when subjected to contact angle of less than 4◦ , which give a self-cleaning character to the
impacts from water and sand, as well as when heated at high tempera­ surface. Moreover, the surface was able to maintain this self-cleaning
tures up to 250 ◦ C, without losing its superhydrophobicity and trans­ superhydrophobic character even after 15 cycles of abrasion, wherein
parency. In addition, the coated substrate showed 94% transmittance mechanical damage was applied to the surface. The results showed that
with only a 3% difference from the uncoated glass. Chemical and me­ the coating could recover its superhydrophobic properties after being
chanical stability tests were carried out on the coating, and the results destroyed by a simple immersion of the surface in DMF, thanks to the
showed that the surface has very excellent chemical stability. It was able presence of intelligent chains of poly(2-perfluorooctylethyl methacry­
to maintain its superhydrophobicity even after immersion in a NaCl late) on the surface. Zian et al. [177] combined ATRP treatment with UV
solution (10% wt) for 48 h. The coating also showed better stability curing to manufacture a superhydrophobic surface. First, the resin ma­
when subjected to impacts from water and sand, as well as when heated trix was mixed with ATRP initiators at different proportions, ranging
at high temperatures up to 250 ◦ C, without losing its super­ from 3% to 15% by weight. Then, the mixture was placed on a glass slide
hydrophobicity and transparency. To test the performance, the coating and exposed to a UV chamber for 10 s to initiate the hardening process.
was applied to photovoltaic cells for two months, and the results showed Next, a superhydrophobic surface was created by grafting a fluorine-rich
that the power conversion efficiency was only reduced by 14.81%. In chain onto the surface using ATRP treatment. Finally, the surface was
comparison, the use of cells without the coating showed a reduction of cleaned and dried. The effect of the amount of initiators on the contact
21%, which is of great importance for the long-term use of solar cells. angle was investigated. It was found that the contact angle varied pro­
Using the same technique, Thongrom et al. [175] made a transparent portionally with the increasing amount of initiators. At a ratio at 6%, the
superhydrophobic coating using the PECVD method and PDMS as a surface began to exhibit superhydrophobic character, and at 15%, the
cover material. The coating was deposited in a single step with a speed of surface showed a maximum contact angle of 174◦ . This result was in
less than 10 s thanks to the high density of electrons in the plasma agreement with the results of SEM. It was noticed that the increase in the
(Fig. 30). It was noted that the variation in deposit time leads to a quantity of initiators leads to the formation of more lumps on the sur­
variation in transmittance. The surface presented a contact angle of 170◦ face, making it more hierarchical. However, for the surface SHS- 6 with a
and sliding angle of 3◦ . 6% surface ratio, a uniform distribution of lumps was observed on the
Despite the success of this technique in producing highly transparent surface compared to the other surface. On the other hand, the poly­
superhydrophobic coatings with excellent self-cleaning and mechanical merization time has an impact on the variation of the contact angle. The
stability properties, its major drawback is the difficulty in scaling up the surface showed the highest contact angle after 6 h of polymerization.
process and its costly synthesis. Furthermore, the superhydrophobic surface SHS-6, treated for 6 h with
ATRP (SHS-6-6), showed excellent chemical stability in different solu­
tions with varying pH, without any loss of superhydrophobicity. This

Fig. 30. Schematic diagram of a custom MW-PECDV system used [175].

20
B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

makes it an ideal base for preparing slippery liquid infused porous sur­
face (SLIPS), which has a lower slip angle than the SHS-6-6 surface and
enhances its self-cleaning properties. Moreover, the transmission of the
two surfaces has been studied, and it has been noticed that the surface of
SLIPS-6 showed 80% better transmittance than the SHS-6 surface, which
exhibited only 30%. In another study, Zan hua et al. [178] created a
transparent surface that can switch between superhydrophobicity and
superhydrophilicity by exchanging ions. First, a glass slide was
immersed in a solution of trichloromethylsilane in the presence of water
and toluene to cover the glass surface with a layer of silicone nanofila­
ments. Subsequently, the glass slide was washed and treated with Fig. 32. The wettability can be switched between superhydrophobicity and
plasma for 30 min. Then, an ATRP control polymerization of 2-(meth­ superhydrophilicity via counterion exchange between Cl− and PFO− [178].
acryloyloxy)ethyltrimethylammonium and trifluoroethanol monomer
was carried out on the surface. Finally, the surface attached to the
copolymer was immersed in a methanol solution containing NaCl or
NaPFO, depending on the desirable surface wettability state (Fig. 31).
The surface showed a transmittance of more than 70%, and it was
observed that the time of polymerization has a significant effect on the
transparency of the coated glass. For a time of polymerization of 1 h, the
transparency is not too much impacted in comparison with the bare
glass. However, with more than 1 h of polymerization, the transmittance
decreases significantly. Moreover, for a time of polymerizations, the
surface showed a contact angle of 164◦ in the case where PFO is used as a
counter-ion. However, when Cl is used as a counter-ion, the surface
shows a contact angle of 3◦ (Fig. 32. This transition between super­
hydrophilic and superhydrophobic, depending on the type of coun­
terion, can be carried out successfully even after numerous cycles
(Fig. 33).
Compared to the methods discussed earlier, direct-to-surface poly­
merization is a versatile and highly effective technique for preparing
transparent self-cleaning surfaces. This technique allows for a wide va­ Fig. 33. Reversible change in wettability on the copolymer-tethered rough
glass surface via counterion exchange for many cycles [178].
riety of vinyl monomer choices with low dispercity while controlling the
molecular weight of the polymers on the surface. Although it has many
advantages, this technique is limited to the laboratory scale due to its primarily due to their self-cleaning properties. However, their applica­
expensive costs. Despite the diversity of methods used for preparing tion on an industrial scale is very limited due to high industrial re­
superhydrophobic coatings, challenges still need to be resolved. quirements, particularly with regard to sustainability and profitability.
To summarize this part, Table 4 presents a summary of the different In general, the main challenges can be summarized in three areas.
methods discussed in this review for preparing superhydrophobic
coatings, including WCA, water rolling angle, and light transmission of - Roughness and transmission: It is well known that roughness and
the coatings. transmission are two contradictory parameters. Ann increase in
roughness leads to a reduction in transmission, while an increase in
6. Challenges and recommendation transmission requires a reduction in roughness and consequently a
decrease in the wettability of the surface. As previously discussed,
The manufacturing of a transparent superhydrophobic coating offers most of the coatings prepared reduce the transparency of the glass
many advantages for improving the production of photovoltaic energy, surface, limiting their application in the fields that require higher
transmittance, such as photovoltaic panels. However, some studies

Fig. 31. Schematic illustration of the fabrication of the transparent coating on a glass substrate by polymerization on the surface [178].

21
B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

Table 4 hydrophobicity or hydrophilicity. Some coatings have shown

Method summary for preparing superhydrophobic coatings. promising thermal stability, but until now, most superhydrophobic
Method Material Contact Sliding Transmittance Ref coatings have not demonstrated sufficient durability to be used in
Angle Angle practice. Mukesh Kumar Meena et al. [179] fabricated a super­
(deg) (deg) hydrophobic coating using functionalized SiO2 nanoparticles by
Spray-coating Silicone resin >150 <10 80% 119 HDTMS in combination with PU polymer by the spin-coating
+ SiO2 method, and the surface showed a contact angle of 165◦ with a slip
Spray-coating SiO2 160 <10 91,03% 120 angle of 7◦ . The coating presented interesting thermal stability up to
Spin-coating PDMS + SiO2 158 80% 121
175 ◦ C without loss of the anti-wetting properties, but after anneal­
<10
Dip-coating MTMS + 171 <10 91% 122
PMMA ing at 200 ◦ C, the surface became hydrophobic due to the melting of
Dip-coating SiO2 + PMMA 174 2 85% 123 the PU resin and the decomposition of HDMS leading to the filling of
Spray-coating PU-PMMA + 165 <10 80% 124 the grooves and reducing the roughness. Although several coatings
SiO2
have shown the ability to withstand high temperatures above 200 ◦ C
Dip-coating PS + SiO2 162 3 91,80% 125
Spin-coating PS + Zn 152 3 91,90% 126 for days, most superhydrophobic coatings have not yet demonstrated
Spray-coating PDMS + 165 3 83% 127 sufficient durability to be put into practice.
Carbon
nanotubes Another external factor that poses a problem for the applications of
Spray-coating SiO2 163 80% 128
superhydrophobic coatings is humidity. It has been shown that when the
<10
Spin-coating PS + SiO2 172 80% 129
Spray-coating Silicone resin 153 9 91,40% 130 coatings are exposed to an environment with higher relative humidity,
+ SiO2 condensation easily occurs on nano-rough structure of the surface
Spin-coating SiO2 + GPDF 160 <10 93,60% 131 forming nucleated microdroplets, which increase the adhesion force of
Spray-coating PFA + SiO2 170 86% 132
the water droplets on the surface, giving the surface a pinned appear­
Spin-coating SiO2 150 5 95% 133
Spray-coating SiO2 150 <10 Good 25 ance. Yin et al. [180] prepared a superhydrophobic coating with a slip
Spray-coating SiO2 + 166 <10 Good 134 angle of 160◦ using the chemical etching method. This coating was
Cerakote placed in humilities of 90%, 60%, and 30%, respectively, and their
Dip-coating SiO2 157,9 <10 98% 135 contact angles were measured at an interval temperature ranging from
Spin-coating Al2O3 161 95% 136
10 to 30 ◦ C. The authors found that at a temperature of 10 ◦ C, super­
<10
Spin-coating SiO2 147 99% 137
Sol-gel SiO2 164 <10 80% 140 hydrophobicity was lost when the humidity was above 60%.
Sol-gel Silica NPs 150 <10 90% 142
Sol-gel Silica sol 150,4 <2 96% 143 - The cost and industrial feasibility: despite the existence of several
Sol-gel Silica sol 162 1,5 95,50% 144
techniques for the manufacturing of superhydrophobic coatings,
Sol-gel TiO2 + OTS 158 4 Good 145
Sol-gel Silica 154 9 89% 146 most of the techniques mentioned require difficult conditions and
alcoholsol somewhat complicated procedures. Furthermore, many of these
Etching SiO2 + 170 <10 Good 152 techniques are very expensive and they are applicable only on small
Methylphenyl surfaces with specific geometries.
silicone
Lithography PDMS 162 3 90% 154
Lithography PET, PMMA, 160 2 Good 155 Based on these three obstacles, four recommendations were
FEP proposed.
Lithography PDMS 150 <10 Good 156
Lithography PUA + PDMS 146 80% 158
- To design durable superhydrophobic coating, it is necessary to ach­
CVD EGDA + PFDA 150 2 94% 167
CVD Epoxy + Silica 154 3,2 87% 168
ieve the formation of covalent bonds between the surface and the
sol + SiO2 coating while obtaining a hierarchical surface with a roughness of
CVD MTMS 165 3 90% 169 less than 100 nm. It has also been observed that a dual-scale
CVD PDMS 170 0 90% 170 microstructure improves the durability of coatings. A new genera­
AACVD MPS + TEOS 167 90% 171
tion of coatings has begun to attract the attention of researchers more
<10
+ POTS
AACVD SiO2 + TTIP + 168 3 90% 172 and more in recent years, these are coatings with nanopores that
PDMS combine a nanoporous structure filled with vacuum with a micron
AACVD PTFE 168 1 92% 173 structure provides roughness. These coatings generally exhibits
PECVD SiO2 153 94% 174
<10
longer lifespan and higher transmittance compared to randomly
PECVD PDMS 170 3 Good 175
Polymerization METAC + 164 3 >80% 178
deposited coatings.
TMA - Self-cleaning coatings have been a trend in recent years due to their
physical and chemical properties which allow them to reproduce
surface properties and superhydrophobicity after their loss. Several
have presented coatings that can maintain o even improve the initial studies have shown that materials such as PDMS, PS, PMMA, have
transparency of the surfaces, although their production can be the ability to prepare self-healing superhydrophobic that can regain
expensive. their superhydrophobic character several times under the effect of an
- Durability: Mechanical and chemical stability is one of the most external stimulus. This leads to the extension of the life of the coat­
crucial factors to validate the effectiveness of self-cleaning coatings ings for a long time.
on an industrial scale, especially since these coatings intended for - The environmental impact must also be taken into consideration
solar energy will be in direct contact with various external factors during the design of superhydrophobic coatings. To achieve low
that can threaten the nanostructure and lead to the loss of super­ surface energy, the majority of the reagents used are known to
hydrophobicity. For example, UV rays and sand can cause the seriously pollute the environment, and they cannot be mass-
destruction of the resin polymeric bonds, which hold the nano­ produced even if they offer high transmission and durability. It is
particles together and result in the loss of the rough nanostructure. necessary to avoid using non-environmentally friendly materials
High temperature can also reduce the performance of coatings and such as fluorinated molecules and replace them with organosilanes
lead to an irreversible change from superhydrophobicity to to ensure that the environmental impact is minimized.

22
B. Nomeir et al. Solar Energy Materials and Solar Cells 257 (2023) 112347

7. Conclusion 2 A good coating must perform well under any conditions it may
encounter when exposed to a given site. For solar panels, they are
The property of self-cleaning is a key solution to solving the problem often exposed to more aggressive and difficult meteorological envi­
of cleaning solar panels, as it can reduce the cost, time and labor ronments than other applications. Therefore, the coatings must have
required to clean solar panels from dust, which is one of the biggest good mechanical durability to ensure a long-term service life. Un­
problems causing a decrease in energy production from solar panels. fortunately, most of the coatings currently available do not have
However, the application of self-cleaning coatings for PV panels not only strong mechanical stability, which can be a major drawback. In the
requires a superhydrophobic surface but also be high transparency and coming years, it is recommended to focus on the development and
mechanical stability, which can be a real challenge to combine all three use of self-healing materials that can repair themselves chemically or
properties. In this review, the manufacturing methods of super­ structurally without the need for external stimulation.
hydrophobic transparent coatings for solar energy applications are 3 To minimize secondary pollution, it is advisable to avoid using non-
presented, by discussing and comparing the various characteristics of environmentally friendly materials. It is logical to encourage
the materials and the methods of preparation used. There will be reducing consumption of fossil resources and replacing them with
interesting and novel properties that will be highlighted. Additionally, renewable energy sources. Additionally, proposing coatings that can
we aim to shed light on various approaches taken by researchers, the add more pollution to the environment should be avoided. Therfore,
challenges encountered, and especially to attract the attention of new it is strongly recommended to manufacture superhydrophobic sur­
researchers in this field who find themselves on the edge of the abyss in faces without fluorine in the coming years and use materials with low
understanding the role of different methodologies and chemistries in the carbon content to reduce carbon emissions in the atmosphere.
development of transparent superhydrophobic coatings. This will help
them to select the best ways of synthesis according to desired final CRediT authorship contribution statement
properties, as briefly concluded below.
Brahim Nomeir: Writing – review & editing, Writing – original
1 It has been found that highly transparent superhydrophobic surfaces draft, Validation. Sara Lakhouil: Supervision. Sofia Boukheir: Visu­
require the combination of two conditions. Firstly, the use of mate­ alization, Project administration. Mustapha Ait Ali: Software, Data
rials with very low surface energy. Secondly, a hierarchical surface curation, Conceptualization. Sanae Naamane: Methodology.
morphology with a fairly high roughness. However, the roughness
must be lower than 100 nm to have acceptable optical properties Declaration of competing interest
acceptable for the field of solar energy, with a transmission rate over
80%. The authors declare that they have no known competing financial
2 The methods commonly used for manufacturing self-cleaning struc­ interests or personal relationships that could have appeared to influence
tures with well-controlled characteristics such as morphology, the work reported in this paper.
roughness, and coating thickness, while maintaining high trans­
parency, are CVD, modeling, and engraving. However, these Data availability
methods have limitations as they can only be carried out on a labo­
ratory scale and are not suitable for large-scale industrial production. No data was used for the research described in the article.
In contrast, solution deposition techniques like spray-coating and
dip-coating offer a fairly simple experimental process, sometimes References
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